Nian Sun, Northeastern University
Jane Chang, University of California, Los Angeles
Shashank Priya, The Pennsylvania State University
Eckhard Quandt, University of Kiel
EL03.01: Multiferroics I
Monday AM, December 02, 2019
Hynes, Level 1, Room 101
8:30 AM - EL03.01.01
Potential of SrTiO3-Based 2DEG for Spin-Charge Interconversion
Unité Mixte de Physique CNRS/Thales1Show Abstract
While classical spintronics has traditionally relied on ferromagnetic metals as spin generato Classical spintronics traditionally relied on ferromagnetic metals as spin generators and detectors. A new approach called spin-orbitronics exploits the interplay between charge and spin currents enabled by the spin-orbit coupling in non-magnetic systems. We studied the potential of the bidimensional electron gases (2DEG) that forms at the interface between LaAlO3 and SrTiO3  or by deposition of Al on SrTiO3 by sputtering . We exploited the sizeable Rashba spin-orbit coupling of the gas to obtain a very large spin-current to charge-current conversion through the inverse Edelstein effect [2, 3]. The efficiency of the conversion, characterized by the Inverse Edelstein effect length, lIEE, is larger than the one measured for the topological insulator a-Sn or at Bi/Ag interfaces . Moreover, this conversion efficiency can be highly modulated by a gate voltage. We used angle-resolved photoemission spectroscopy and Boltzmann calculations to map this peculiar gate dependence and linked it to the band structure. We will show that the conversion process is amplified by enhanced Rashba-like splitting due to orbital mixing, and in the vicinity of avoided band crossings with topologically non-trivial order . This suggest that oxide interfaces have a strong potential for spin-based information readout in novel memory such as the magneto-electric spin-orbit transistor proposed by Intel.
 E. Lesne et al., Nat. Commun. 5, 4291 (2014) ; D. C. Vaz et al., Adv. mat. 29, 1700486 (2017).
; D. C. Vaz et al., Nat. Mat. (2019)
 E. Lesne et al., Nat. Mat. 15, 1261 (2016)
 J.-C. Rojas-Sánchez et al., Nature Com. 4, 2944 (2013) ; PRL 116, 096602 (2016).
 S. Manipatruni et al., Nature 565, 35 (2019)
9:00 AM - EL03.01.02
Chiral Domain Topology, Moire Patterns and Magnetism in Intercalated Transition Metal Dichalcogenides
Sang Wook Cheong1
Rutgers Univ1Show Abstract
Transition metal dichalcogenides (TMDs) have been extensively investigated as 2D materials last decade. A large amount of transition metals (M) can be intercalated into the van der Waals gaps of a wide range of TMD materials, but a limited recent studies in intercalated TMDs have been reported. The limited examples include FexTaS2 crystals with x=1/4 and 1/3, which exhibit intriguing configurations of antiphase and/or chiral domains related to the ordering of intercalated M ions with 2a×2a and √3a×√3a superstructures, respectively. In addition, Cr1/3NbS2 undergoes helical spin order below 133 K, and shows an interesting soliton-lattice behavior when in-plane magnetic fields are applied in the helical spin state. We have explored a series of chiral M1/3Ta(Nb)S(Se)2 to investigate the correlation among crystallographic symmetries, magnetic domain topologies and their physical properties. These results as well as Moire patterns with self-twisted TMDs induced by intercalation will be discussed.
9:30 AM - EL03.01.03
Multiferroics—Hidden Functionalities beyond Magnetoelectric Coupling
ETH Zurich1Show Abstract
Requirements to "good multiferroics" are tough. They are supposed to have a spontaneous magnetization and polarization, preferably parallel to each other, with a strong magnetoelectric coupling between them. Inevitably, this leads to a multiferroic state that is described by a very complex set of order parameters – complex enough to provide the symmetry degrees of freedom to fulfil so many requirements at once . With the focus on electric-field-controlled magnetic order, it may go unnoticed that these degrees of freedom will permit many functionalities other than bulk magnetoelectric coupling. In my talk, I will describe the quest for such functionalities in our group. This includes inversion of a ferroelectric or a ferromagnetic multi-domain state in a homogeneous electric or magnetic field: In each domain, the direction of the order parameter is reversed but the domain pattern as such is left untouched . In addition, a ferroelectric domain pattern on a uniformly magnetized background is transduced into a ferromagnetic domain pattern on a uniformly polarized background. Finally, a multiferroic bulk state is "condensed" into a multiferroic domain wall in a non-multiferroic environment.
 M. Fiebig et al., Nature Rev. Mater 1, 16046 (2016)
 N. Leo et al., Nature 560, 466 (2018)
10:30 AM - EL03.01.04
New Concepts for the Direct Conversion of Heat to Electricity Using Multiferroics
University of Minnesota1Show Abstract
We describe recent progress on materials and devices for the direct conversion of heat to electricity applicable to the small temperature difference regime, 10-200 C. This regime includes abundant natural and waste heat sources, but there is currently no reasonable method to harvest the energy. We are pursuing an idea based on the use of first order phase transformations with either an abrupt change of magnetization or polarization at the transformation. In the ferromagnetic case the electricity is harvested by induction; in the ferroelectric case, by capacitance. It is a “direct” method in the sense that there is no separate electrical generator. We survey the theory of this method, the design of the materials and devices, and the analysis of various cycles. We compare theoretical predictions and the behavior of a prototype under cyclic heating/cooling. These devices provide interesting possible ways to recover the vast amounts of energy stored on earth at small temperature difference. They move heat produced by natural and man-made sources from higher to lower temperature and therefore contribute negatively to global warming. This lecture draws on work with Kanwal Bhatti, Ashley Bucsek, Xian Sherry Chen, Bharat Jalan, Bill Nunn, Yintao Song and Vijay Srivastava.
11:00 AM - EL03.01.05
Electric Field-Controlled Magnetism in (Bi,R)FeO3 Solid Solutions
Xiang Ming Chen1,Jing Chen1,Xin Xin Shi1,Bin Xu2,Ting Ting Gao1,Laurent Bellaiche3
Zhejiang University1,Soochow University2,University of Arkansas3Show Abstract
BiFeO3 has attracted the increasing scientific attention as the most important room temperature single phase multiferroic material. However, the weak magnetoelectric coupling in BiFeO3 seriously obstructs its applications. The cycloidal spin structure is actually a hint of the existence of the magnetoelectric coupling. In the present work, the magnetoelectric coupling has been realized by destroying the cycloidal state and switching it to the weak ferromagnetic state through symmetry modulation. Electric field-controlled magnetism is achieved in Bi1-xRxFeO3 solid solutions by tuning the symmetry from polar R3c to polar Pna21, where two morphotropic phase boundaries (MPB) are detected together with the greatly enhanced ferroelectric polarization and magnetism. The electric field-controlled magnetism is realized by an electric field induced structural transition from Pna21 back to R3c which results in the magnetic transition from weak ferromagnetic state to cycloidal state, and this transition is shown to be reversible with additional thermal treatment.
11:30 AM - EL03.01.06
Coexistence of Multiferroicity and Metallic Conductivity in One-Dimensional Single-Component Radical
Yong Hu1,Shenqiang Ren1
University at Buffalo1Show Abstract
Multiferroics and metallic conductivity seem mutually exclusive and cannot be obtained in one material. Dielectric property requires the localized charge and the electrical conducting behavior is based on the free charge carriers. The confined electronic structure in one-dimensional (1D) materials might break this long-standing contradiction. Electrons confined to a 1D chain exhibit various instabilities followed by symmetry breaking, such as superconductor, topological insulator and multiferroics. Here we report the discovery of laser shock induced insulator-metal transition in K-TCNQ radical, where the effect of antiferromagnetic spin ordering causes dipole ordering. The manipulation of spin exchange interaction with external laser shock wave, electric field and magnetic field is accompanied by insulator to metal transition, gigantic magnetoelectric and magnetocapacitance effects, respectively. Therefore, 1D systems with strongly coupled multiple degrees of freedom of electrons-spin, charge, and orbital-provide a new area to search for conducting magnetoelectric media. Our study opens the way for electron engineering, symmetry breaking and establish of self-organized electronic order from modular building blocks, permits the rational design of functional electronic materials that exhibit technologically useful behaviour.
 E. Coronado, J. R. Galan-Mascaros, C. J. Gómez-García, V. Laukhin, Nature 2000, 408, 447.
 J.-K. Bao, J.-Y. Liu, C.-W. Ma, Z.-H. Meng, Z.-T. Tang, Y.-L. Sun, H.-F. Zhai, H. Jiang, H. Bai, C.-M. Feng, Phys. Rev. X 2015, 5, 011013.
 G. Autès, A. Isaeva, L. Moreschini, J. C. Johannsen, A. Pisoni, R. Mori, W. Zhang, T. G. Filatova, A. N. Kuznetsov, L. Forró, Nat. Mater. 2016, 15, 154.
 A. S. Tayi, A. K. Shveyd, A. C.-H. Sue, J. M. Szarko, B. S. Rolczynski, D. Cao, T. J. Kennedy, A. A. Sarjeant, C. L. Stern, W. F. Paxton, Nature 2012, 488, 485.
 R. Kumai, Y. Okimoto, Y. Tokura, Science 1999, 284, 1645.
11:45 AM - EL03.01.07
Spintronics with Magnetoelectric Antiferromagnetic Thin Films
Denys Makarov1,Tobias Kosub1
Helmholtz-Zentrum Dresden-Rossendorf e.V.1Show Abstract
Thin film magnetoelectric antiferromagnets (AF) have potential to revolutionize spintronics due to their inherently magnetic-field stable magnetic order and high-frequency operation. To explore their application potential, it is necessary to understand modifications of the magnetic properties and magnetoelectric responses of AF thin films with respect to their bulk counterparts.
Our approach is based on the electron transport characterization of magnetic responses of thin film antiferromagnets [1-4]. This task is difficult as minute uncompensated surface magnetization of antiferromagnets needs to be detected, which imposes strict requirements to the sensitivity of the method. We will outline our developments of zero-offset anomalous Hall magnetometry  applied to study the physics of insulating magnetoelectric Cr2O3 antiferromagnets. To build a reliable description of the material properties, the analysis of the transport data is backed up by structural characterization and real space imaging of AF domain patterns using NV microscopy [1,2]. Considering grainy morphology of thin films, we address questions regarding the change of the intergranular exchange , criticality behavior and switching of the order parameter .
The fundamental understanding of the magnetic microstructure of magnetoelectric α-Cr2O3 thin films and the possibility to read-out its antiferromagnetic order parameter all-electrically enabled the entirely new recording concept where a magnetoelectric memory cell can be addressed without using a ferromagnet, the purely antiferromagnetic magnetoelectric random access memory (AF-MERAM) . In addition to the outline of the memory concept, we discuss on the physics of the readout signal in α-Cr2O3 interfaced with Pt .
 T. Kosub et al., Nat. Commun. 8, 13985 (2017).
 P. Appel et al., Nano Letters 19, 1682 (2019)
 T. Kosub et al., Phys. Rev. Lett. 115, 097201 (2015).
 R. Schlitz et al., Appl. Phys. Lett. 112, 132401 (2018).
EL03.02: Magnetoelectrics I
Monday PM, December 02, 2019
Hynes, Level 1, Room 101
1:30 PM - EL03.02.01
Recent Progress in Spintronics for Energy Efficient Systems
Kang Wang1,Armin Razavi1,Hao Wu1
University of California, Los Angeles1Show Abstract
Spintronic devices take advantage of the nonvolatility of magnetism and electrical control high energy efficiency, and thus offer promise to deliver next-generation systems in memory and computation as well as RF devices and systems. Spintronic devices offer the advantages of non-volatility, low switching energy (< fJ), high speed/frequency (<10 ns), and an almost unlimited endurance (>1016). The development of this technology is especially crucial in the advent of big data and artificial intelligence, which demand fast access to large amounts of data at high processing speeds. In particular, recent advances on memory (magnetic random-access memory, MRAM) and logic devices have also drawn interest in memory-centric computing paradigms. In this talk, we will first provide an overview of the progress of magnetic materials for high spin orbit coupleing (SOC) and spin orbit torque (SOT) applications. We will discuss SOC and magnetoelectric effects as two routes for energy efficient MRAMs. In SOT systems, a high spin-SOC material is used to create a tranverse spin current to manipulate or switch the magnetic moment of an adjacent magnet through a torque in a magnetic tunneling junction device (MTJ). We will discuss recent advances in SOTs, including the applications of topological insulators surface states for increasing the switching energy efficiency. A major challenge for SOT switching is that it requires an additional inversion symmetry breaking to become deterministic, which is usually provided by applying an in-plane external magnetic field. We discuss the recent progress for realizing field-free deterministic SOT switching through symmetry breaking using various techniques, including antiferromagnetic materials and structural symmetry breaking.
Second, we will highlight progress in synthetic layered materials to achieve magnetoelectric effects for memory and logic devices using the voltage-controlled magnetic anisotropy (VCMA) effect, very much like multiferroic mateirals. In this case, a voltage is applied across the magnetic tunnel junction to reduce the anisotropy energy barrier to allow for the voltage controlled switching of the free layer in an MTJ but with a thicker MgO barrier layer, instead of of passing current through the MTJ. VCMA devices are two-terminal and have a much higher density compared to SOT structures which require three terminals for read/write. The reduction of energy barrier per unit voltage is characterized by the VCMA coefficient; to improve the effectiveness of voltage control and scaling to high densities, it is necessary to improve the VCMA coefficient > 1,000 fJ/Vm (first 1,000 challenge). We discuss the recent progress in this area, with a focus on interface and seed/spacer/insertion engineering. For this and related MTJ devices, the readout uses a tunneling magnetoresistance ratio (TMR). The state of the art TMR is of 200~300%. For improved read operation a large signal-to-noise ratio for readout in large arrays, TMR > 1,000%, is desirable and warrant as the second 1,000 challenge. We show strategies for enhancing TMR based on using materials with high spin polarization, such as Heusler alloys. Another challenge for VCMA devices is their high write-error-rate, which can be mitigated by using circuits-based approaches or new device concepts (such as skyrmion-mediated switching). The similar concepts may be applied to energy efficient RF systems. Lastly, for THz applications, ferrimagnetic and antiferromagnetic materials for enhancing the operation speed/frequency will also be briefly disussed.
2:00 PM - EL03.02.02
Thin Film Magnetoelectric Composite Sensors—Sensitivity and Bandwidth at Low Frequency
Kiel University1Show Abstract
Composite materials consisting of magnetostrictive and piezoelectric constituents are known for efficient strain mediated magnetoelectric (ME) coupling. Magnetic field sensors made out of such composites yield high sensitivity and low detection limits in the pT field range. Thin film ME sensors reach sensor performance similar to that of their bulk material counterparts provided that the frequency of magnetic field coincides with a mechanical resonance frequency of the sensor structure. In general this condition is not fulfilled. The measurement of e.g. biomagnetic signals requires extremely low detection limits at frequencies of few Hertz and a minimum bandwidth in the order of 20 Hz.
This presentation considers three different ME sensor concepts to enhance sensitivity to low frequency signals, i.e. magnetic frequency conversion (MFC), surface acoustic wave (SAW) sensors, and piezoelectrically driven sensors based on converse ME effect and inductive read-out by a surrounding pick-up coil. The focus is on designing the magnetostrictive phase, which must be tuned to the sensor concepts differing in underlying effects, utilized substrate, sensor size and thickness, as well as operating magnetic or piezoelectric excitation. In MFC the ME sensor structure is exposed to strong modulating magnetic fields changing the magnetization of the magnetostrictive film periodically with a frequency of about 1 kHz. In contrast to that, the converse ME effect sensors are piezoelectrically driven at comparably high frequencies (515 kHz). The SAW sensors are operated by means of interdigital transducer electrodes at 146 MHz leading to mechanical wave propagation at the device surface and thus through the magnetoelastic phase. Utilizing the ΔE effect, phase change between input and output signal serves as a measure of the applied field. With regard to the various concepts, the interplay between magnetic configuration, associated magnetic noise, and resultant ME sensor performance is investigated.
All sensors are fabricated by bulk micromachining. The sensors for MFC and converse ME effect are of Si cantilever type with 2 µm thick AlN serving as piezoelectric phase. The cantilevers are 350 µm thick and have lateral dimensions of 2.2 mm x 25.2 mm. Enabled through the thin film approach and magnetron sputter deposition, single FeCoSiB and complex multilayers comprising up to 80 individual layers form the magnetostrictive phase. The multilayers consist of repetitions of the stacking order unit Ta 5 / Cu 3 / MnIr 8 / FeCoSiB x [thickness in nm] with varying thickness x of the FeCoSiB layer. The total thickness of the FeCoSiB layers adds up to 1 µm, 2 µm, and 4 µm.
The SAW sensors are based on single crystal Quartz substrates with a 4.5 µm thick silicon oxide layer functioning as guiding layer for horizontal shear waves. Single FeCoSiB layers with a thickness ranging from 25 nm to 750 nm are deposited on the guiding layer and in between the transducers. SAW sensor sensitivity and insertion losses are investigated in dependence on the FeCoSiB layer thickness.
At current status, similar detection limits ranging between 60 pT/Hz1/2 and 150 pT/Hz1/2 are observed at 10 Hz frequency for all three kinds of sensor concepts. However, converse ME effect sensors and SAW sensors benefit from wider bandwidth of about 1 kHz and 1 MHz, respectively.
The presented work was conducted within the framework of the Collaborative Research Center CRC 1261, funded by the German Research Foundation (DFG).
2:30 PM - EL03.02.03
Novel RF NEMS Magnetoelectric Resonators for Sensors, Neville Sun Show Abstract
3:30 PM - EL03.02.04
Synthesis of Coaxial Nanofibers of Hexagonal Ferrites and Ferroelectrics and Studies on Strain Mediated Magneto-Electric Interactions
Gopalan Srinivasan1,Ying Liu1,2,Peng Zhou2,Wei Zhang1,Tianjin Zhang2
Oakland University1,Hubei University2Show Abstract
We report on the synthesis of coaxial nanowires of ferrimagnetic hexagonal ferrites and ferroelectric lead zirconate titanate (PZT) or barium titanate (BTO), assembly of nanostructures into superstructures with the aid of magnetic and/or electric fields, and studies on the nature of coupling between the magnetic and electric subsystems . Such multiferroic nano-composites are expected to show strong strain mediated magneto-electric (ME) coupling due to very high surface area-to-volume ratio . The efforts were on fibers of Y- or W-type hexagonal ferrite and PZT or BTO and their assemblies. Core-shell fibers with (Ni, Zn) Y-type or (Co, Zn) W-type hexaferrites and ferroelectrics were prepared by electrospinning. The choice of Zn-substituted ferrites with planar or uniaxial anisotropy was aimed at control of magnetic order parameters for ME studies at low frequencies and at resonance modes of electric and magnetic subsystems and over a wide frequency range, from 1Hz to 110 GHz. The fiber synthesis was carried out by dispensing sol gels of ferrites and ferroelectrics through a coaxial syringe with a dual syringe pump. It was possible to control the core and shell diameters by controlling the gel viscosity, strength of the electric field and core and shell diameters of the needle. Electron-, scanning probe-, and scanning microwave microscopy of fibers annealed at 700-900 C showed fibers of shell diameter 200-800 nm and core diameter of 50-200 nm with well defined core-shell interface. Fibers were characterized in terms of magnetic, ferroelectric, and electromagnetic parameters. The magnetization for the fibers were in general agreement with values for bulk ferrites, but the polarization was one to orders of magnitude smaller than expected values. Investigations on ME effects were performed on 2D and 3D fibers assembled in a magnetic field and on discs of the fibers annealed at high temperatures. Low-frequency ME voltage coefficients (MEVC) for the films and discs were in the range 0.3 to 3 mV/cm Oe with the highest values measured for fibers of (Ni, Zn) Y and PZT. Magnetic field assembled films showed a higher MEVC than unassembled films. Polarization P vs electric field E measurements under an applied static magnetic field H on discs indicated a fractional change in the remnant polarization as high as 7% for H = 7 kOe. Magneto-dielectric measurements on films at 12-26 GHz showed 2-3 % fractional change in the dielectric permittivity for H = 7 kOe. The nanofibers studied in this work show strong ME coupling and are of interest for application in sensor and energy harvesting technologies.
The research was supported by a grant from the NSF (DMR-1808892)
1. D. Viehland, J. F. Li, Y. Yang, et.al., J. App. Phys.124, (2018): 061101.
2. V. Petrov, J. Zhang, H. Qu, et.al., J. Phys. D: Appl. Phys. 51, 284004 (2018).
4:00 PM - EL03.02.05
Smart Magnetoelectric Antennas for Magnetic Sensing and Energy Harvesting
Mohsen Zaeimbashi1,Mehdi Nasrollahpour1,Xianfeng Liang1,Huaihao Chen1,Anthony Romano1,Ziyue Xu1,Ankit Mittal1,Nikita Mirchandani1,Gaurav Jha1,Isabel Martos-Repath1,Adam Khalifa2,Marvin Onabajo1,Aatmesh Shrivastava1,Sydney Cash2,Nian Sun1
Northeastern University1,Massachusetts General Hospital, Harvard Medical School2Show Abstract
Recent progress in the field of magnetoelectric (ME) materials have led to ultra-compact ME antennas with size of 2-3 order of magnitude smaller than that of conventional state-of-the-art compact antennas . These miniaturized antennas could be suitable for Medical Implant Communications Service (MICS), in particular for wireless brain monitoring. A wireless implantable device should be able to perform multiple tasks in order to effectively monitor an individual’s condition. For instance, a wireless implantable device should harvest their required energy in order to power their circuitry systems. In addition, the implant needs to record the body’s information such as magnetic or electric fields in order to successfully track the changes the body. Finally, the implant should transmit the recorded data to the external antenna or device.
In this work we’re presenting an ultra-compact and smart magnetoelectric antenna that can single-handedly perform all three above-mentioned tasks: energy harvesting, magnetic field sensing, and data communication. This complimentary combination makes ME antennas suitable for brain implantation where magnetic field recording is required to monitor the brain functionality. Fig. 1 shows the optical microscope image of fabricated ME antenna with AlN/FeGaB thin-film structure. AlN acts as a piezo-material and FeGaB as a magneostrictive material. Proposed antenna has three parallel ME element, each with the size of 50×250 µm2. Fig. 2a shows the architecture of energy harvesting setup. Fig. 2b shows the ME antenna concept and its functionality in receiving (energy harvesting) mode. Fig. 2c shows the S11 of ME antenna showing the resonant frequency of 2.25GHz. Fig. 2d shows the harvesting voltage from ME antenna, showing an induced voltage of 2.13mV when ME antenna is in presence of a 4.5nT RF magnetic field. Fig. 3a shows the ME antenna’s phase response in magnetic sensing mode. Here, ME antenna is in presence of a 1kHz magnetic field with 6.6µT strength. Fig. 3b is the zoomed-in version of Fig. 3a and shows the 1kHz phase peak which corresponds to the 6.6µT magnetic field under measurement. The limit of detection of this antenna is 917pT.
 T. Nan, H. Lin, Y. Gao, A. Matyushov, G. Yu, H. Chen, et al., "Acoustically actuated ultra-compact NEMS magnetoelectric antennas," Nature communications, vol. 8, p. 296, 2017.
4:15 PM - EL03.02.06
Charge-Lattice and Spin-Lattice Interactions in Multiferroics and Magnetoelectrics
Brookhaven National Laboratory1Show Abstract
Topological structures and defects including ferroelectric and ferromagnetic vortices emerging near spontaneous symmetry-breaking transitions are ubiquitously observed in wide branches of science. They are invariant under continuous deformations, or perturbations, and protected by topology, thus are promising candidates as information carriers for future memory and logic devices. However, their controlled manipulation including creation and annihilation remains an important challenge towards practical applications. In this presentation I will give a few examples. 1) Structural transformation of sixfold ferroelectric vortex domains into crystallographically forbidden two-, four-, and eightfold vortices via a second topological defect in hexagonal manganites. Combining high-resolution electron microscopy and Landau-theory-based numerical simulations, we investigate the remarkable atomic arrangement and the intertwined relationship between polarization and topological defects. 2) Controlled evolution of helical and skyrmion phases in multiferroic oxides as function of doping, temperature, and magnetic field from direct imaging using in-situ Lorentz phase microscopy. We reveal that skyrmion channeling effectively suppresses the second skyrmion phase formation at low temperature, envisaging designing of skyrmion flow circuits based on multiferroic thin films for spintronics. If time allows, other material systems will also be presented.
Collaborations with S. Cheng, J. Li, and MG. Han at BNL and Jan Seidel at UNSW are acknowledged. Work at BNL was supported by DOE/BES-MSD under Contract DESC0012704.
4:45 PM - EL03.02.07
Emission and Active Manipulation of Spin Waves in Multiferroic Heterostructures
Sebastiaan van Dijken1,Huajun Qin1,Sampo Hämäläinen1
Aalto University1Show Abstract
Multiferroic heterostructures comprising strain-coupled ferromagnetic and ferroelectric layers can be exploited as programmable hybrids in magnonics. Attractive properties of multiferroic heterostructures include the imprinting of magnetic domain patterns with a regular modulation of magnetic anisotropy, the creation of abrupt anisotropy boundaries, strong pinning of straight magnetic domain walls, and electric field control of magnetic anisotropy, magnetic switching, and magnetic domain wall motion [1-3]. Here we show that these attributes provide an attractive platform for the emission of short-wavelength spin waves , the confinement of spin-wave modes in structurally uniform films , and the manipulation of spin-wave transmission . In our studies, the multiferroic heterostructures consist of a ferroelectric BaTiO3 substrate and a strain-coupled ferromagnetic film with a thickness of 20 – 50 nm. At room temperature, this material system comprises fully correlated stripe domains in the ferroelectric and ferromagnetic subsystems. Utilizing strong pinning of ferromagnetic domain walls onto ferroelectric boundaries, we demonstrate active manipulation of spin wave transmission from ~0% to ~100 % by non-volatile reprogramming of the domain-wall spin structure in a magnetic field . We also present results on electric field control of spin wave transmission using local domain switching via lateral wall motion in perpendicular electric fields. Many of the magnonic concept realized in multiferroic heterostructures are extendable to other material systems with regular modulations of magnetic anisotropy.
 T. H. E. Lahtinen, J. O. Tuomi, and S. van Dijken, Adv. Mater. 23, 3187 (2011).
 T. H. E. Lahtinen, K. J. A. Franke, and S. van Dijken, Sci. Rep. 2, 258 (2012).
 K. J. A. Franke, B. Van de Wiele, Y. Shirahata et al., Phys. Rev. X 5, 011010 (2015).
 B. Van de Wiele, S. J. Hämäläinen, P. Baláz, F. Montoncello, and S. van Dijken, Sci. Rep. 6, 21330 (2016).
 S. J. Hämäläinen, F. Brandl, K. J. A. Franke, D. Grundler, and S. van Dijken, Phys. Rev. Appl. 8, 014020 (2017).
 S. J. Hämäläinen, M. Madami, H. Qin, G. Gubbiotti, and S. van Dijken, Nat. Commun. 9, 4853 (2018).
EL03.03: Poster Session I: Multiferroics and Magnetoelectrics
Monday PM, December 02, 2019
Hynes, Level 1, Hall B
8:00 PM - EL03.03.01
Electronic and Magnetic Transitions in LaNiO3-δ Nickelate Perovskites with Ordered Oxygen Vacancies
Yongjin Shin1,James Rondinelli1
Northwestern University1Show Abstract
Rare-earth nickelates perovskites (RNiO3, with R=rare earth) are of high academic interest as they show sensitive variability in their properties with subtle structural changes. Unlike other RNiO3 compounds, LaNiO3 is the only compounds showing no metal-insulator transitions with temperature as the relatively large size of La suppresses the distortive mode stabilizing insulating phase. Instead, LaNiO3-δ exhibits interesting electronic/magnetic transitions with varying oxygen contents δ. Specifically, the metal-semiconductor-insulator transition occurs concurrently with paramagnetic (PM)-ferromagnetic (FM)-antiferromagnetic (AFM) transition in bulk materials . The origin of these transitions can be associated with ordered oxygen-vacancies in LaNiO3-δ, which transforms NiO6 octahedra to NiO4 square planer units along (110)p direction. As the square planar units are with different coordination environment and crystal-field splitting of d-orbital states, the assembly of two units results in unique electronic/magnetic structures.
In this work, we investigate the role of ordered-oxygen vacancies in LaNiO3-δ by using first-principles calculations on LaNiO3-δ phases with δ=0, 0.25, and 0.5. The LaNiO2.75 is composed of octahedral slabs separated by square planer plane, while LaNiO2.5 is with a columnar arrangement of square planes and octahedra. We show that the magnetic properties of LaNiO3-δ are mainly determined by octahedral units with limited connectivities, as Ni2+ on square planer unit is with low-spin configuration and magnetically inactive. We also explain the structural distortions induced by insertion of square planer units, and conclude by connecting our findings to experimental bulk properties.
 R.D. Sanchez, M.T. Causa, A. Caneiro, A. B. Metal-Insulator Transition in Oxygen-Deficient LaNiO3-x Perovskites. Phys. Rev. B 1996, 54 (23), 574–578.
8:00 PM - EL03.03.02
Enhanced Magnetoelectric Properties and Structural Phase Transition in BiFeO3:YbEr Thin Films
Ratnakar Palai1,Ricardo Martinez Valdes1,Claudia Zuluaga1,Blanca Rosas1,Javier Wu1,Ram Katiyar1,Shawn Zografos1,Hannu Huhtinen2,Wojciech Jadwisienczak3
University of Puerto Rico1,University of Turku2,Ohio University3Show Abstract
Multiferroics materials are scientifically and technologically promising because of their potential applications in multi-state memory for data storage, magnetic recording, spintronics, quantum electromagnets, and sensors. BiFeO3 (BFO) is one the rare single-phase room temperature multiferroics and shows ferroelectricity up to 820oC and antiferromagnetism below 370oC. However, high leakage current, weak magnetoelectric coupling, presence of cycloidal spin spiral, and critical structural stability of BFO are the bottlenecks for practical applications. Rare earths show many Interesting optoelectronic and magnetoptic properties. In order to enhance the magnetoelectric properties, we investigated Yb and Er co-doped BFO [Bi1-2x(YbxErx)FeO3] ( x = 0.05, 0.10, 0.15, 0.2, and 0.25) bulk and thin film samples. We found that samples with x =0.1 and 0.15. Samples with 20 and 30% rare earth show significant improvement in magnetoelectric properties with very high polarization (~ 100 µc/cm2). The enhanced magnetic properties can be explained by the localization of 4f electrons and high effective magnetic moments of rare earth. A structural phase transition has been observed above 20% doping of rare earth. The effect of co-doping of rare earth on enhanced magnetoelectric properties and phase transition will be discussed in detail.
8:00 PM - EL03.03.03
A Study on the Multiferroic Properties of Bi- and Tri-Layer Hydrogenated Graphene
Solimar Collazo1,Samuel Escobar1,Rajesh Katiyar1,Ernesto Espada1,Vladimir I. Makarov1,Brad Weiner1,Gerardo Morell1
University of Puerto Rico at Río Piedras1Show Abstract
Hydrogenated graphene has been of great interest for the scientific community due to properties like ferromagnetism and piezoelectricity that are not usually present in graphene; requiring subsequent functionalization after synthesis to obtain them. Hereby, we present a novel method for synthesizing hydrogenated graphene via a single-step process. Hydrogenated graphene was characterized primarily by Raman spectroscopy, X-ray Photoelectron Spectroscopy (XPS), X-ray Diffraction spectroscopy (XRD) and Physical Properties measurement system (PPMS). Our Raman spectra confirms the presence of the 2930 cm-1peak associated with hydrogen functionalization, while the PPMS reveals the strongest ferromagnetism at room-temperature of a carbon-based material with a curie temperature higher than 350 K. Preliminary research also suggests the presence of ferroelectricity within our material. These results are strong evidence of hydrogenated graphene’s capabilities for its implementation to spintronics & memory applications.
8:00 PM - EL03.03.06
Dynamics of Phase Transition and Spin-Phonon Coupling in Ho2Ti2-xO7- δ
Ratnakar Palai1,Karuna Mishra1,Ricardo Martinez Valdes1,SM Koohpayeh2
University of Puerto Rico1,Institute for Quantum Matter, Johns Hopkins University2Show Abstract
A2B2O7 pyrochlores are of great scientific interest because of their interesting magnetic orderings (spin-liquid, spin-ice state, Neel-order) and crystal structure. Rare earth pyrochlores shows Ising-like spins, frustrated ferroelectricity, and multiferroic behavior. Pyrochlores also have the ability to immobilize actinides, thus could be used for the disposal of nuclear waste. We report on dielectric, electrical conductivity, magnetic behavior of pyrochlore Ho2Ti2-xO7- d (x = 0.0 and ± 0.08) down to 5 K . For the better understanding of dynamics of phase transition and spin-phonon coupling, we employed micro-Raman spectroscopic studies of phonon spectra from 82 K- 700 K. Magnetic excitation induced phonon renormalization is evident in the low temperature magnetic phase. The presentation will discuss the results in details.
8:00 PM - EL03.03.07
Room Temperature Lead Palladium Titanate Nanoscale Multiferroic Thin Films
Karuna Mishra1,Mohan Bhattarai1,Ram Katiyar1
University of Puerto Rico1Show Abstract
The discovery of single-phase magnetoelectric materials and their analysis of coupling mechanisms between spin and polarization is important from the point of view of next generation logic and memory devices. Herein, we report fabrication, dielectric, ferroelectric and magnetic measurement of a Pd-doped room-temperature magnetoelectric multiferroic PbPd0.3Ti0.7O3 (PbPdT) thin film. Highly oriented PbPdT thin films were deposited on (LaAlO3)0.3(Sr2AlTaO6)0.7 substrates by following laser ablation processes in oxygen atmosphere using pulsed laser deposition technique. Diffraction studies revealed that the film had tetragonal phase with (001) orientation. The surface morphology studies using atomic force and scanning electron microscopic techniques suggest a smooth and homogeneous distribution of grains on the film surface with roughness ~2 nm. The dielectric measurements as a function of temperature were carried out in Pt/PbPdT/LSMO metal-dielectric-metal capacitors that showed diffused behavior over a large range of temperatures at several frequencies, and exhibited a higher dielectric constant ~3200 at room temperature. The measured polarization hysteresis loops at room temperature were attributed to its ferroelectric behavior. A well-saturated magnetization M-H loop with remanent magnetization of 3.5 emu/cm3 was observed at room temperature. The origin of magnetization is argued on the mixed oxidation states of Pd2+/Pd4+ in the PbTiO3 matrix and complemented by x-rays photoelectron spectroscopic experimental results. These results suggest that our thin films are multiferroic (ferroelectric-ferromagnetic) at room temperature. The details will be presented in the meeting.
8:00 PM - EL03.03.08
Electrical and Magnetic Properties of Thin Single Crystal Cr2O3 Films
Nguyen Vu1,Xiangpeng Luo1,Steve Novakov1,Wencan Jin1,Johanna Nordlander2,Peter Meisenheimer1,Morgan Trassin2,Liuyan Zhao1,John Heron1
University of Michigan1,ETH Zürich2Show Abstract
Magnetoelectric materials have been of great interest due to their potential for low-power spintronic devices via the electric field switching of magnetization. Antiferromagnet Cr2O3 is one of a very few room temperature magnetoelectrics and possesses unique properties such as uncompensated surface spins and perpendicular magnetic anisotropy.  Since the first demonstration of the electric field control of exchange bias in bulk single crystal Cr2O3 heterostructures , intense effort has focused the demonstration of magnetoelectric switching using Cr2O3 thin films at room temperature. [3,4] The existence of twin domains in thin films grown on metallic electrodes, however, leads to high leakage current and dielectric breakdown fields that can only be circumvented by growing rather thick films (250-500 nm). [4,5] By using an isostructural epitaxial oxide electrode, V2O3, recent studies have shown the reduction and even possible elimination of twin domains in Cr2O3 films.  Dielectric and magnetoelectric switching studies of 200 nm thick films show bulk like performance, however, for next generation logic and memory the films must be scaled down. 
Here we present an investigation of the electrical endurance and magnetic properties of very thin (30-60 nm) single crystal Cr2O3 films grown by pulsed laser deposition onto V2O3 buffered (0001) oriented Al2O3 substrates. Our results show that 60 nm single crystal thin film has bulk-like resistivity ( 1012 cm) and significantly improved breakdown voltage (150-300 MV/m). Using magnetometry, we investigate exchange bias of thin film Cr2O3/ferromagnet heterostructure. The blocking temperature is found to be at 285 K which is higher compared to twinned films with similar or greater thickness in literature.  Further, Second Harmonic Generation confirms bulk magnetoelectric order of our single crystal thin film at room temperature. These results indicate the importance of crystallinity to realize bulk like properties in very thin films at room temperature.
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 T. Kosub, M. Kopte, R. Hühne, P. Appel, B. Shields, P. Maletinsky, R. Hübner, M. O. Liedke, J. Fassbender, O. G. Schmidt, and D. Makarov, Nat. Commun. 8, 13985 (2017).
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 N. Shimomura, S. P. Pati, T. Nozaki, T. Shibata, and M. Sahashi, AIP Adv. 7, 025212 (2017).
8:00 PM - EL03.03.10
Multifferroic Behavior in Na0.5Bi0.5-xEuxTiO3
Ratnakar Palai1,Ricardo Martinez Valdes1,S. Behara2,P. Kuruva2,T. Thomas2,Wojciech Jadwisienczak3
University of Puerto Rico at Río Piedras1,IIT Madras2,Ohio University3Show Abstract
The complex perovskite Na0.5Bi0.5TiO3 (NBT) is a promising lead-free piezoelectric with interesting ferroelectric (Tc = 670 K) property and phase transition. The unusual A-site positional disorder and relexor ferroelectric behavior in NBT makes it an important material for practical applications. Rare earth doped perovskites show interesting magneto-optic and opto-electronic properties. In order to develop a room temperature magneto-electric multiferroic material, we explored Eu-doped NBT Na0.5Bi0.5TiO3 (NBT:Eu) with different concentrations. In this paper we report on optical, dielectric, ferroelectric, magnetodielectric, and magnetic properties NBT:Eu prepared by solid-state reaction. The as-synthesized NBT:Eu materials have Eu concentration between 1 to 20 at.% using A-site substitution in the general ABO3 perovskite oxide are single phase, polycrystaline materials as determined by powder X-ray diffraction study . The luminescence intensity monitored at 617 nm increases linearly with the Eu concentration increase up to 20 at.% without indication of typically observed concentration quenching effect. The photoluminescence (PL) and cathodoluminescence (CL) spectra are dominated by sharp characteristic emission lines corresponding to Eu3+ intra-4fn shell transitions centered at 593 nm (5D0→7F1), 617 nm (5D0→7F2) and 700 nm (5D0→7F4), respectively. The PL excitation spectroscopy reveal that optically active Eu3+ ion centers can be effectively excited with photons between 325 nm to 550 nm via energy migration or direct resonant excitation processes. The electron paramagnetic resonance shows that characteristic electron spin resonance signal of Eu2+ ions are not observed in these material. The crystal field calculations and temperature dependent PL and CL studies have shown that the luminescence of Eu3+ ions occupying centro-symmetric and non-centro-symmetric sites; however corresponding luminescence temperature thermal quenching mechanisms are different for photon- and electron-excited spectra. Recently studied dielectric permittivity, dielectric loss, impedance, and phase angle of NBT:Eu as function of frequency  were correlated with corresponding magnetic properties of the NBT:Eu subjected to up to 1 Tesla. It was found that material shows a novel room temperature ferromagnetic like behavior, which is unusual, but can be explained by the local structural disordering or phase coexistence. Finally, we will discuss the defects in NBT:Eu and their effect on observed optical, electric and magnetic properties of this novel multifferroic material.
 R. Prusty, P. Kuruva, U. Ramamurty, T. Thomas, Sol. State Commun., 173 (2013) 38-41.
 A. Kalaskar, B. Narayana Rao, T. Thomas, and R. Ranjan, J. Appl. Phys. 117 (2015) 244106.
8:00 PM - EL03.03.11
Heterointegration of Complex-Oxide Epitaxial Films
Hyunseong Kum1,Hyungwoo Lee2,Sungkyu Kim1,Shane Lindemann2,Chang-Beom Eom2,Jeehwan Kim1
Massachusetts Institute of Technology1,University of Wisconsin–Madison2Show Abstract
To date, physical coupling of complex-oxide materials has been predominantly demonstrated through epitaxial means, which limits the breath of possible combinations of materials and restricted by lattice mismatch conditions between the epitaxial layer and substrate. Therefore, there is an increasing trend across all functional single-crystalline materials to lift-off the epitaxial layer from the substrate and transfer the membrane onto foreign substrates. This not only opens up immense amount of freedom to integrate various functional materials on one platform, it also potentially allows reuse of expensive and exotic substrates, expediting commercialization. To this end, we have developed a method to generate freestanding complex-oxide membranes by growing on top of graphene as well as precise cleaving at an epitaxial interface. This allows us to transfer and stack arbitrary complex-oxide membranes which was not possible by epitaxial means, allowing us to study new oxide interfaces and coupling phenomena.
We exfoliated several single-crystalline complex oxide films (e.g. SrTiO3, CoFe2O4, Y3Fe5O12 etc.) by growing them on top of graphene coated substrates. The graphene layer acts as a slippery exfoliation layer which allows crystal growth but also epitaxial lift-off1,2. Additionally, we have found that it is possible to exfoliate single crystalline PMN-PT from STO surface with atomic precision. PMN-PT has one of the highest piezoelectric coefficients, and also shows exotic properties such as high pyroelectricity which has only started to be investigated3. Not only were we able to exfoliate the films, we were able to reuse the substrate several times to continuously produce freestanding oxide membranes using a single substrate.
Using these films, we were able to fabricate a freestanding multiferroic bilayer laminate (CFO/PMN-PT), where CFO is a magnetostrictive material and PMN-PT is a piezoelectric material. We compared the magnetoelectric coupling of our freestanding device to a device not exfoliated from the substrate. An order of magnitude larger signal could be measured for the freestanding device compared to the device still clamped to the substrate, which demonstrate the applicability of our method.
8:00 PM - EL03.03.12
Effective Voltage Control of Resistance Modulation in VO2 by Gating through Hexagonal Boron Nitride
Hidekazu Tanaka1,Yuto Anzai1,Mahito Yamamoto1,Teruo Kanki1,Kenji Watanabe2,Takashi Taniguchi2
Osaka University1,National Institute for Materials Science2Show Abstract
Phase transitions in transition metal oxides, such as metal-Insulator transition, ferromagnetic, ferroelectric materials, are useful phenomena to realize novel electrical/magnetic switching and sensing devices. Among them, the strongly correlated electron system of VO2 exhibits an ultrafast metal-insulator transition (MIT) under external stimuli. If the MIT in VO2 can be controlled by a voltage, a field effect transistor (FET) could be demonstrated with ultrafast and ultralow power consumption switching properties. Here, to enhance the resistance modulation in VO2 FETs, we employ, as a gate insulator, a layered material of hexagonal boron nitride (hBN) which is atomically flat and has much fewer electron trap sites than the other gate oxides have. The VO2 thin film with a thickness of 10 nm was grown on TiO2 by the pulsed laser deposition method and, then, was etched down to 5 micrometer in width. The thickness of hBN was 30nm as top gate geometry. This VO2 thin channel undergoes a metal-insulator transition at around 325 K in the heating process. The transfer curve and gate leakage current of the VO2 FET was measured at 310 K (the drain bias V d is 1.0 V). The drain current increased clearly when applying the positive gate voltage (electron doping), while the current decreased under the application of the negative gate voltage (hole doping). We find no hysteresis and memory behavior in the VO2 FET under gating, indicating no chemical reactions and trapping at the interface. This gate-response speed was observed to be faster than the measurement limit of 400 ms. Namely, a slow response caused by the carrier trap at the interface was not observed. We also investgated the stability of the hBN gate insulator under gating. We can find that the drain current rarely changes during the application of the gate voltage for 3000sec. These observations show that hBN is a chemically and electrically stable material for the gate insulator application. The resistance of VO2 was modulated by up-to 1.2% at a gate voltage of 20 V, which is 4 times larger than in previously reported VO2 FETs with oxide gate insulators such as SiOx. This is likely because with hBN the interface carrier scattering is strongly suppressed. Our results indicate the advantage of use of h-BN as 2D material in order to demonstrate voltage control of transition metal oxides via electrostatic modulation.
8:00 PM - EL03.03.19
A Potential Multiferroic Material—Co Doped Hf0.5Zr0.5O2
Zimeng Zhang1,Xiaoxi Huang1,Vishal Thakare1,Vishal Ravi1,Yen-Lin Huang1,Ramamoorthy Ramesh1
University of California, Berkeley1Show Abstract
There is currently quite a bit of interest in multiferroics and magnetoelectrics for low power electronics. While there have been many new multiferroics added to the well-studied BiFeO3 system, most of them have transition temperatures below room temperature. Thus, discovering new multiferroic and magnetoelectrics is desirable. Doped magnetic ferroelectrics (DMFE) are attracting attention in this regard since many of them have to potential to multiferroic/magnetoelectric property at room temperature. One such model system is BaTiO3 doped with magnetic impurities. Our strategy is to take well known ferroelectrics, such as Hf0.5Zr0.5O2 (HZO) and introduce magnetic impurities, such as cobalt into the lattice. Prior work on Co-doping of TiO2 has revealed interesting magnetic effects and that forms the backdrop for our work. HZO is a simple fluorite showing robust ferroelectricity at the nanoscale and good compatibility with silicon and hence is a favored candidate for the next generation memory and logic devices. HZO has many phases, among which orthorhombic and rhombohedral phases possess ferroelectricity. Using epitaxy as the underlying driver, we have been able to demonstrate high quality HZO thin films in the 1-20nm thickness range. Doping with 5% Co does show the existence of a magnetic moment. We are presently studying the effects of Co concentration on the magnetic and ferroelectric stability. We demonstrated the existence of ferroelectricity by PFM and P-E loop measurements and tested the magnetic hysteresis loops. We will present results of this investigation on the role of HZO crystallinity and Co-doping on the magnetoelectric properties.
8:00 PM - EL03.03.20
Magnetodielectric Properties of Co/PZT/Co Spin Capacitor
Ratnakar Palai1,Fernando Aponte1,Roberto Masso-Ferret1,Ricardo Martinez Valdes1
University of Puerto Rico at Río Piedras1Show Abstract
Spin capacitors have the potential to store both the electronic charge and magnetic spin that can produce conventional electric current and spin polarized current. The time evolution of spin polarized electrons injected into the piezoelectric material can be used for accurate sensing of magnetoelectric fields. To further study the application of multiferroic spin capacitors for future use in memory applications, Ferromagnetic/Ferroelectric/Ferromagnetic tri-layer artificial multiferroelectric structures in spin capacitor configuration were fabricated. Previous experiments were done by sputtering Iron (Fe) and Nickel (Ni) electrodes on lead zirconate titanate (PZT). In this paper, we report dielectric, magnetic, and magnetoelectric coupling in the tri-layer composite with Cobalt (Co) as the magnetic electrode sputtered onto PZT polycrystalline of different thickness. Various dielectric measurements were carried out, including: capacitance, impedance, loss coefficient, dielectric permittivity, and phase angle measurements done by a wide range of frequencies (100 Hz – 5 MHz) and magnetic fields (0 Tesla – 2.0 Tesla) at room temperature, and their interaction with the presence of the applied magnetic field (magnetocapacitance and magnetoimpedance) were analyzed. We also compared the magnetodielectric measurements of the Co/PZT/Co spin capacitor with Co/PZT/Ag and Ag/PZT/Ag tri-layers structures with their respective their behaviors. The magnetodielectric studies of different PZT layer thickness will be discussed in details.
8:00 PM - EL03.03.22
Magnetic and Dielectric Properties of Potential Multiferroic GdCrO3
Jianhang Shi1,Yanliu Dang1,Steven Suib1,Menka Jain1
University of Connecticut1Show Abstract
Multiferroics materials have attracted a lot of attention due to their potential technological applications. GdCrO3 that belongs to the family of rare-earth chromites (RCrO3) has recently been reported to be a single phase magnetoelectric multiferroic. However, the origin or existence of ferroelectricity in GdCrO3 remains ambiguous. We have, therefore, examined the properties of bulk and thin film samples to explore their multiferroic properties. Magnetic measurements have revealed that it shows an antiferromagnetic transition with weak ferromagnetism below the Néel temperature TN 169 K as well as spin reorientation, and giant magnetocaloric effect (MCE) at lower temperatures. In this work, structure, particle size, substitution effect, magnetic, and dielectric properties of this family of material will be presented.
8:00 PM - EL03.03.23
Invstrigation of Interface Structure in Multiferroic h-ScFeO3 Film
Yosuke Hamasaki1,Shintaro Yasui2,Takahisa Shiraishi3,Akihiro Akama3,Takanori Kiguchi3,Tomoyasu Taniyama4,Mitsuru Itoh2
National Defense Academy1,Tokyo Institute of Technology2,Tohoku University3,Nagoya University4Show Abstract
Polar iron oxides, which exhibit both ferroelectricity and (anti)ferromagnetism, are multiferroic materials, which promises potential application for new type memory devices. Hexagonal ReFeO3 (h-ReFeO3) (Re = Rare earth element) with YMnO3(YMO)-type structure exhibits ferroelectricity and weak-ferromagnetism. First principle calculation revealed that h-ReFeO3 exhibits improper ferroelectricity (geometric ferroelectricity). Due to the strong magnetic interactions between Fe3+ cations, the higher magnetic order temperature in h-ReFeO3 compared with hexagonal manganites is expected. A magnetic phase transition temperature of h-ReFeO3 increases with decreasing ionic radius of Re cation. h-ReFeO3 which consists of small ionic Re cation is a candidate for a high temperature multiferroic material.
Metastable h-ReFeO3 were obtained by containerless melt crystallization process and crystallization from amorphous phase. Masui et. al. prepared Sc substituted LuFeO3 by containerless process, and h-Lu1-xScxFeO3 was obtained in the range of x = 0 - 0.8. h-ReFeO3 (Re = Tb-Lu, Y ) were stabilized on substrates such as YSZ(111) and Pt(111)/Al2O3(0001) in film form by pulsed laser deposition (PLD) and sputter techniques. Previously, we stabilized h-ScFeO3 film on an Al2O3(0001) substrate using PLD technique. However, preparation of h-ScFeO3 have not been reported yet. In this study, we attempted to prepare h-ScFeO3 film on electrodes and investigated their physical properties and interface structure.
h-ScFeO3 was deposited on various electrodes such as ITO, ZnO, SrRuO3, and (La,Sr)MnO3 by PLD technique. Single phase h-ScFeO3 was obtained on La0.8Sr0.2MnO3//SrTiO3(111). Crystal structure of film was characterized by X-ray diffraction (XRD) and scanning transmission electron microscope (STEM). XRD measurements and HAADF-STEM observation revealed that h-ScFeO3 with YMO-type structure was epitaxially grown with the relationships of ScFeO3(0001)//La0.8Sr0.2MnO3(111)//SrTiO3(111).
The YMO-type ScFeO3 film showed a ferroelectric P-E hysteresis loop with Pr ~ 4.9 μC/cm2 and weak ferromagnetism with TN = 195 K. The TN value is the highest in hexagonal ReFeO3 and ReMnO3. Interface studies revealed that the monolayer consisted of two paired Sc cations connected to the YMO-type and perovskite structures. One of two paired Sc cations was displaced upward because of Coulomb repulsion from the Mn cations of La0.8Sr0.2MnO3. We deposited ScFeO3 film on various perovskite films or substrates. Single phase h-ScFeO3 film was obtained on perovskite films or substrates with low valence B site cations. This results indicated that the valence of B cations in perovskite played an important role in the formation of the interface monolayer.
8:00 PM - EL03.03.25
Magnetic and Magnetocaloric Properties of Pd Doped in FeRh Alloy with Large Refrigerant Capacity
Yafen Shang1,2,Yutao Cao1,Ravi Hadimani3,Yurij Mozharivskyj2,Hao Fu1
University of Electronic Science and Technology of China1,McMaster University2,Virginia Commonwealth University3Show Abstract
The B2-orderd intermetallic magnetic compound FeRh exhibits a thermodynamically first-order phase transition in vicinity of room temperature that makes it a highly intriguing subject for both fundamental and applied study. The structure, magnetic, and magnetocaloric properties of Pd doped in FeRh alloy have been investigated. Experiments revealed that there are same structures type FeRh (CsCl-type) with different lattice parameters and Fe15.7Rh (bcc-W type) phases are coexist in FeRh0.95Pd0.05 sample. The wide phase transition temperature range is about 250 K, which is from 150 K to 400 K for this alloy. The maximum magnetic entropy change (-ΔSM) is 16.6 J/kg K for 0 - 30 kOe field changes and refrigerant capacity (RC) of 1347 J/kg was obtained due to the contribution of large transition temperature range. The excellent magnetocaloric performance indicates the applicability of FeRh0.95Pd0.05 as an appropriate candidate for magnetic refrigerant.
8:00 PM - EL03.03.26
Magnetic Properties of Co3-XNiXO4 (0 ≤ X ≤ 1.28) Particles Synthesized from Co1-YNiY(OH)2 Precursors
Kensuke Hayashi1,Keisuke Yamada1,Mutsuhiro Shima1
Gifu University1Show Abstract
Magnetic properties of cobalt nickel spinel oxides Co3-XNiXO4(CNO) have been extensively studied over decades [1,2]. In the Co-Ni-O system, CNO is known to be metastable under atmospheric conditions as the rock-salt phase (Co1-YNiYO) is stable when T > 1173 K while NiO and Co3O4 phase are stable when T ≤ 1173 K . Due to CNO’s metastability, it is believed to be difficult to chemically synthesize CNO for X > 1 through conventional process such as thermal decomposition and co-precipitation [2,4]. CNO thin films grown by physical vapor deposition for X > 1[5,6], reportedly yield relatively low Curie temperatures (TC = ~100-200 K for X = 1) in contrast to higher TC for powder CNO (TC = ~400 K) . Recently, it was reported that CNO samples for X > 1 can be synthesized by thermal decomposition of organic metal frameworks (MOF) for super capacitor electrodes applications . In this case, CNO for X > 1 can be synthesized from Co-Ni MOFs where Co and Ni ions are uniformly mixed at an atomic scale. In this study, we report successful synthesis of CNO particles for X = 0-1.28 from Co1-YNiY(OH)2 precursors in which Co and Ni ions are uniformly mixed at an atomic scale, and the magnetic properties of the CNO at room temperature.
[Experimental] The Co1-YNiY(OH)2 precursors were prepared from a hydrochloric aqueous solution containing Co2+ and Ni2+ by a uniform precipitation process. They were the annealed at 573-873 K for 3 hours in the air to transform into CNO particles. Their magnetic properties were investigated by vibrating sample magnetometry (VSM), electromagnetic resonance (EMR) spectrometry, and superconducting quantum interference device (SQUID) magnetometry at temperature from 5 K to room temperature (RT).
[Results and Discussion] X-ray diffraction spectrometry (XRD) of the samples have shown that CNO particles are successfully synthesized for X ≤ 1.28 without producing any other phases. The lattice parameter of CNO increases linearly with increasing X, yielding with Vegard’s law. The mean particle size of CNO estimated from XRD data using Scherrer’s equation is 8~33 nm. Magnetic measurements by VSM show that CNO particles for X ≥ 0.74 possess remanent magnetization and coercivity at RT, it reveals that the CNO particles are ferrimagnetic at RT. Microwave absorption peaks are observed in the ENR spectra of CNO particles for X ≥ 0.74. The EMR spectra of the CNO samples exhibit absorption peaks best fitted only by the Gaussian function. The peaks can generally be fitted by the Gaussian when it contains a ferromagnetic (ferrimagnetic) component and/or the Lorentzian when it has a paramagnetic one in the sample. Hence, it is suggested that the ferromagnetic CNO samples possess a fairly high crystallinity with few defects breaking magnetic interaction in the crystal. SQUID measurements of the samples shows that their saturation magnetization increases with increasing X for X < 0.74 and decreases for X ≥ 0.74.
 S. Chikazumi, Physics of Magnetism (Shokabo, Tokyo, 2001) 18th ed.,Vol. 1, p. 225 [in Japanese].  F. K. Lotgering., Philips Res. Rep. 11, 337 (1956).  R. J. Moore, et al., J. Mater. Sci. 9, 1393, (1974).  S. Kuboon, et al., Ind. Eng. Chem. Res. 50, 2015, (2011).  J. S. McCloy, et al., J. Phys. Chem. C. 119, 22465, (2015).  Y. Bitla, et al., Sci. Rep. 5, 15201, (2015).  S. Chen, et al., J. Mater. Chem. A. 3, 20145, (2015).
8:00 PM - EL03.03.29
Probing the Ferromagnetic Resonance of the Si/Ge2Sb2Te5/FeCoB Heterostructures Induced by Phase Change
Yuyi Wei1,Xinjun Wang1,Jiawei Wang1,Nian Sun1
Northeastern University1Show Abstract
Over the past few decades, phase change materials (PCM) has received a lot of attention for its application such as novel non-volatile memory,[1-4] switches[5,6] and sensors. Typically, PCMs exist in an amorphous and one or more crystalline phases, in which significant optical and electrical contrast can be observed. The change in state can be rapidly and repeatedly switched by inducing optical pulses or electrical (Joule) heating.[8,9] In 2011, F. Xiong et al. proposed a low power switching using GST with programming current of 1 to 8 µA and programming voltage of below 1V, indicating an energy loss of femtojoules scale. This design not only brought a promising prospect to ultra-low power electronics and memory development but also proposed inspiration in voltage control of ferromagnetic resonance (FMR).
Here, a systematic study of the coupling effect in Si/Ge2Sb2Te5/FeCoB heterostructures is presented. We investigated the FMR change in FeCoB film induced by crystalline phase change in GST film. A large shifting in FMR field of 15 mT in FeCoB film can be observed when GST is highly crystallized after annealing at 300 °C. And the uniaxial magnetic anisotropy field is also strengthened when Ge2Sb2Te5 is highly crystallized in hexagonal phase via interfacial coupling effect. With all these results, a novel structure using PCMs for voltage control of FMR is proved to be applicable. This structure can be predicted to have very low operation voltage as well as ultra-low energy consumption, showing an extraordinary advantage in the development novel fast response, energy efficient tunable microwave devices and non-volatile magnetic memory.
8:00 PM - EL03.03.30
Two-Dimensional Transport in LaTiO3 Thin Films Embedded in SrTiO3
Jiyeon Lee1,Mikk Lippmaa1
University of Tokyo1Show Abstract
Oxide materials with unexpected transport and magnetic properties at interfaces have generated great interest in multifunctional heterostructure design. One of the best-known systems is the interface between LaAlO3 and SrTiO3, exhibiting a two-dimensional electron gas in a strongly asymmetric quantum well due to possible switching or spintronic device application. There is growing experimental evidence that the carrier accumulation in a quantum well at the interface leads to magnetic order that may be tunable or switchable if sufficient carrier density control can be achieved. However, except for limited tunability by electrostatic back-gating, it has proven to be difficult to control the carrier density in the electron gas.
In this work, we have chosen to use a similar electronic system consisting of a thin LaTiO3 film, with a thickness of a few unit cells, embedded in SrTiO3. While metallic conductivity at the LaAlO3/SrTiO3 interface appears abruptly when the LaAlO3 film thickness exceeds 4 unit cells, the total carrier number in the LaTiO3/SrTiO3 system is continuously tunable over a wide range by changing the number of La atoms in the LaTiO3 layer. Since the presence of a single LaO layer in the perovskite lattice is sufficient to induce metallic conductivity, a polar discontinuity does not arise, but carriers are still confined in a quasi-2D quantum well and form a high-mobility layer, similar to the LaAlO3/SrTiO3 interface. When the heterostructure is grown on a single crystal SrTiO3 substrate and capped with a SrTiO3 film that is grown at low temperature, the difference in the dielectric permittivities of the substrate and the cap layer leads to an asymmetric quantum well, similar to the LaAlO3/SrTiO3 heterostructures.
By using this specially designed heterostructure, we discuss how to determine the depth distribution of carriers while changing the LaTiO3 or SrTiO3 cap layer thickness and look at the effect of the carrier distribution on the magnetotransport characteristics. Our experiments show that a large negative in-plane magnetoresistance effect occurs at low temperature when the magnetic field is applied parallel to the current, in a qualitatively similar fashion to LaAlO3/SrTiO3 interfaces. We also discuss the effects of back-gating on the magnetotransport characteristics and interpret the results in terms of carrier depth distribution changes in the heterostructure under electrostatic bias. We attempt to distinguish whether the observed negative in-plane magnetoresistance is related to carriers confined at the interface or those that distribute over a larger depth in the substrate-side tail of the quantum well and how such carrier redistribution affects the carrier density in the quantum well.
 A. Ohtomo, and H. Y. Hwang, Nature, 427, 423 (2004).
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 M. Diez, A. M. R. V. L. Monteiro, G. Mattoni, E. Cobanera, T. Hyart, E. Mulazimoglu, N. Bovenzi, C. W. J. Beenakker, and A. D. Caviglia, Phys. Rev. Lett. 115, 016803 (2015).
8:00 PM - EL03.03.32
Investigation of Geometry Parameters Influencing the Performance of Cantilever Magneticelectric Sensors
Jingxiang Su1,Florian Niekiel1,Simon Fichtner1,Christine Kirchhof2,Dirk Meyners2,Eckhard Quandt2,Bernhard Wagner1,Fabian Lofink1
Fraunhofer Institute for Silicon Technology1,Kiel University2Show Abstract
Magnetoelectric (ME) sensors currently have attracted great interest due to their capability to detect magnetic fields in the picotesla regime at room temperature, showing a high potential in the biomagnetic field detection. Based on the magnetoelectric effect of ME sensors, the applied magnetic field induces a change in the strain of magnetotrictive layer which will be transferred to the piezoelectric material via the mechanical coupling. An electrical voltage across the piezoelectric layer is thus generated and can be measured directly. However, for the application of non-invasive medical imaging like magneto-encephalography or -cardiography (MEG, MCG), a magnetic field sensor with a limit of detection (LOD) in the range of picotesla is required. To reach this goal, the LOD of ME sensors still needs to be further improved.
There are many approaches to improve LOD of ME sensors, either by increasing the sensitivity, or by decreasing the intrinsic noise level. A simple solution for improving the sensitivity is to optimize the geometry parameters of the ME sensor through a parameter study. Recent studies have investigated the influence of the geometry parameters of the individual layers and the substrate layer on the sensitivity of cantilever ME sensors using finite element model . Here, an experimental model is built up for determining the basic parameters of the cantilever ME sensor.
In this study, we present cantilever ME sensors based on magnetoelectric composites with various geometry parameters. The cantilever contains poly-silicon layer, piezoelectric material (AlN) and magnetoelectric material (FeCoSiB) in sequence. The performance of the presented sensors is studied based on the sensitivity, voltage noise density, quality factor and LOD. Three different parameters including the cantilever length, the substrate thickness and the thickness ratio between the magnetostrictive and piezoelectric layers are analyzed to understand their effect on sensors’ performance. Since the devices were fabricated in 8 inch silicon technology, the availability of a relavant number of devices allows a statistical analysis. The results are used to identify the optimal geometry parameters for cantilever ME sensors and can be applied to develop next generation devices.
Funding by the DFG via the Collaborative Research Center SFB 1261 is gratefully acknowledged.
 M. C. Krantz, J. L. Gugat and M. Gerken, AIP ADVANCES, 3, 062135 (2013)
 J. L. Gugat, M. C. Krantz and M. Gerken, IEEE Transactions, 49, 5287 (2013)
8:00 PM - EL03.03.33
Lead Free Multiferroic Nano-Heterostructured Films for Energy Storage Applications
Mohan Bhattarai1,Sita Dugu1,Ram Katiyar1
University of Puerto Rico, Rio Piedras1Show Abstract
Lead free environment friendly multiferroic perovskites thin films are of research interest due to its reduction in dimensionality leading to high energy storage and magneto electric behavior and hence are suitable for several electronic device applications. Herein, we report the tetragonal multiferroic heterostructure thin films fabricated by pulse laser deposition technique consisting alternate of Ba(Zr0.30Ti0.70) 0.99 Fe0.01 O3 (BZTF) and Ba(Zr0.30Ti0.70) O3 (BZT) layeres grown upon LSMO coated on MgO (100) substrate. X-ray diffractometry data analysis suggests phase purity of thin films oriented along (100) direction. Micrograph structural analysis using atomic force microscopy revealed a homogeneous distribution of grains with roughness ~ 3- 5 nm. Dielectric measurements on Au/BZT/BZTF/LSMO and Au/BZTF/BZT/LSMO metal insulator metal capacitors using a impedance analyzer as a function of temperature (100-650 K) and frequency (102-106 Hz) suggest their relaxor behavior. The slim P-E loop also corroborate relaxor behavior. The temperature dependent magnetic measurements using a physical property measurement system suggest the existence of magnetic nano clustures dispersed in a paramagnetic matrix and attributed to its super para magnetic behavior. A large energy storage density is estimated from our P-E loop data. These results suggest the present heterostructured thin films could be promising multiferroic materials for high energy density applications.
8:00 PM - EL03.03.35
Ferroelectric-Paraelectric Phase Transition in SnTiO3, a Lead-Free Putative Ferroelectric
Karuna Mishra1,Rajesh Katiyar1,Gerardo Morell1,Brad Weiner1,Ram Katiyar1
University of Puerto Rico, San Juan1Show Abstract
The environmentally benign nature of Sn2+ would make SnTiO3 (SnTO) derived compounds an attractive alternative to lead-free dielectric material. Several theoretical studies suggested that the spontaneous polarization of SnTO is larger than that of classical ferroelectric PbTiO3. Pure phase of SnTO is one of the challenging jobs due to often mixed oxidation states of Sn2+ and Sn4+ in perovskite titanates. The material was synthesized using a chemically route followed by a solid-state reaction method and were annealed it in a mixture ratio of 1:1 methane:hydrogen environment. The phonon spectra of tetragonal ferroelectric SnTO compound were measured as a function of temperatures in the range 82-1250 K using a micro-Raman spectrometer equipped with a CCD detector. Seven phonons are identified in the frequency range 100-1000 cm-1 at the room temperature and are assigned as per the C4v point group symmetry. The reduced temperature dependent spectra were analyzed using the damped harmonic oscillator model to obtain the thermal evolution of the mode frequencies and their intensities. Upon increasing temperature, the optical phonon modes were found to be soften and their intensities decreases, as normally expected, due to involved multi-phonon scattering processes. At 823 K, the A1(TO) phonon located at 441 cm-1, exhibits anomaly and begins to harden upon further increase in temperature; in addition, the E(LO) mode at 827 cm-1 disappear around 823 K, suggesting a tetragonal ferroelectric to a high symmetry paraelectric cubic phase transition. The nature of transition is found to be first order displacive type. The appearance of symmetry forbidden broad Raman bands in the high temperature cubic phase is attributed to contribution from phonon density of states. These studies on phonon behaviors on this putative green ferroelectric could provide insight about its structure-property relations and its thermodynamics properties as well. The detail results will be presented at the meeting.
8:00 PM - EL03.03.36
Temperature-Induced Phase Transitions and Charge Transport in Ferroelectric [KNbO3]1-x[(BaNi1/2Nb1/2O3-δ)]x Electroceramics
Blanca Rosas1,Alvaro Instan1,Karuna Mishra1,Ram Katiyar1
University of Puerto Rico1Show Abstract
Potassium niobate (KNbO3) is a lead-free piezoelectric material, respectful of the environment and technologically very important. This is because it has excellent electromechanical properties and diverse applications in electronic and photonic devices. The electro-physical properties, such as the crystalline phase transition, the optical band gap, the dielectric constant, the Curie temperature, the electrical conductivity and the ferroelectric behavior of KNbO3 can be tuned by suitable dopant, such as isovalent Ba in it’s A-site, and heterovalent Ni on B-site results in a single phase ceramic material with stoichiometric formula [KNbO3]1-x [(BaNb0.5Ni0.5O3-δ)]x for x = 0.1 and δ = 0.25 (KBNNO). The structural, optical, dielectric, charge transport phenomena and ferroelectric properties of this solid solution were systematically investigated. The ceramic material was prepared by the solid-state reaction method and calcined at 1198 K, using starting precursors as K2CO3 (99.5%), BaCO3 (99.95%), Ni2O3 (99.9%) and Nb2O5 (99.9%). The orthorhombic ferroelectric phase formation of the synthesized samples is confirmed by using X-ray diffractometry and Raman spectroscopic analysis. Surface morphology study using scanning electron microscopy revealed well-sintered nature of the sample with grains are interconnected and densified. Temperature-dependent in-situ x-rays diffraction studies (300-873 K) revealed the phase transitions from room temperature orthorhombic to tetragonal to a cubic phase at elevated temperatures. The temperature dependent Raman spectra studies in the T-range 82-1000 K suggest that several bending and stretching phonon mode frequencies and their intensities exhibit anomalous changes across the phase transitions temperatures. These transition temperatures were corroborated with the DSC measurements. A direct optical band gap of 3.16 eV is estimated from the analysis of the diffuse reflectance spectra using Kubelka-Munk analysis. The dielectric properties of KBNNO were studied as a function of temperature between 80-500 K in a frequency range from 100 Hz to 1 MHz in a metal-ferroelectric-metal capacitor nanostructure. The dielectric constant and the loss tangent at 100 kHz were 280 and 0.01, respectively. The frequency dependence of the AC conductivity showed typical characteristics of the universal dynamic response. Our studies reveal the structure-property relation, fundamental physics and materials science of KBNNO electroceramics, and establishing its potential for ferroelectric device applications.
Nian Sun, Northeastern University
Jane Chang, University of California, Los Angeles
Shashank Priya, The Pennsylvania State University
Eckhard Quandt, University of Kiel
EL03.04: Multiferroics II
Tuesday AM, December 03, 2019
Hynes, Level 1, Room 101
8:00 AM - EL03.04.01
Breaking Symmetries to Create a Robust Room-Temperature Ferrimagnetic Ferroelectric in LuFeO3/CoFe2O4 Superlattices
Darrell Schlom1,R. Steinhardt1,M. E. Holtz1,P. Barrozo2,3,4,A. Coleman1,I. Glushchenko1,C. J. Fennie1,D. A. Muller1,5,Ramamoorthy Ramesh3,4
Cornell University1,Federal University of Sergipe, São Cristóvão2,University of California, Berkeley3,Lawrence Berkeley National Laboratory4,Kavli Institute at Cornell for Nanoscale Science5Show Abstract
Materials that exhibit simultaneous order in their electric and magnetic ground states hold tremendous promise for use in next-generation, low-power memory and logic devices in which electric fields control magnetism. Such materials are, however, rare as a consequence of the competing requirements for ferroelectricity and magnetism, and until recently BiFeO3 was the only material with this functionality at room temperature. Interface materials are a way to overcome these competing requirements, as was recently demonstrated for (LuFeO3)m/(LuFe2O4)1 superlattices [J.A. Mundy et al. Nature 537 (2016) 523–527.]. The rumpling imposed by the geometric ferroelectric hexagonal LuFeO3 imposes a local distortion on the neighboring LuFe2O4—a distortion that removes the mirror symmetry that the LuFe2O4 layers would otherwise have. This breaking of symmetry enables the LuFe2O4 to become simultaneously ferrimagnetic and ferroelectric. This rumpling is distinct from strain engineering because no macroscopic strain is involved. In this presentation we extend this atomically engineered design methodology to LuFeO3/CoFe2O4 superlattices producing a robust ground state that is simultaneously ferroelectric and ferrimagnetic at temperatures well above room temperature.
8:30 AM - EL03.04.02
Electric Field Control of Magnetism at Room Temperature
University of California, Berkeley1Show Abstract
There is currently a lot of R&D activity worldwide on two broad, systems level topics, both within the field of Microelectronics. One of them has to do with the emergence of the “Internet of Things”, which is the interconnectivity of microelectronics based sensing, communicating and information processing systems. The second has to do with the re-emergence of Artificial Intelligence/ Machine Learning, which is currently experiencing a worldwide explosion. Thus, the worldwide market for microelectronics is likely to go up significantly. A key side consequence of this is the total energy consumed in such applications, which could sky-rocket towards 20-25% of primary energy and thus of concern. Indeed, in the field of AI, a “Computing Wall” driven by a “Memory Wall” has emerged as a key bottleneck in systems level applications, such as in “Connected Autonomous Vehicles” or driver-less cars. At the same time, the key driver for the field of Microelectronics, namely Moore’s Law, is reaching the end of size scaling and power scaling. As a consequence, there is a large amount of research activity focused on the new Moore’s Law that is instead focused on Energy Scaling. Thus, looking for a new generation of ultra-low power memories and switches is an area of significant current research. Complex perovskite oxides exhibit a rich spectrum of functional responses, including magnetism, ferroelectricity, highly correlated electron behavior, superconductivity, etc. The basic materials physics of such materials provide the ideal playground for interdisciplinary scientific exploration with an eye towards such applications. Over the past decade the oxide community has been exploring the science of such materials as crystals and in thin film form by creating epitaxial heterostructures and nanostructures. Among the large number of materials systems, there exists a small set of materials which exhibit multiple order parameters; these are known as multiferroics, particularly, the coexistence of ferroelectricity and some form of ordered magnetism (typically antiferromagnetism). The scientific community has been able to demonstrate electric field control of both antiferromagnetism and ferromagnetism at room temperature. Current work in our collaboration is focused on ultralow energy (1 attoJoule/operation) electric field manipulation of magnetism as the backbone for the next generation of ultralow power electronics. We are exploring many pathways to get to this goal. In this talk, I will describe our progress to date on this exciting possibility. The talk will conclude with a summary of where the future research is going.
9:00 AM - EL03.04.03
Magnetic Monopoles Hidden in Magnetoelectric Materials
ETH Zurich1Show Abstract
In linear magnetoelectric materials, an electric (magnetic) field induces a magnetization (electric polarization) with a magnitude that is linearly proportional to the applied field strength. Here we use the prototypical magnetoelectric material, Cr2O3, to show that magnetoelectric materials with a diagonal magnetoelectric response host a hidden hedgehog-like magnetic order known as the magnetoelectric monopolization. We describe several consequences of this hidden order: First, we show that the magnetoelectric monopolization leads to a surface magnetization, independently of the choice of surface cut, that in turn should influence the exchange bias coupling in a heterostructure. Second, we show that a charge on the surface of such a magnetoelectric induces a divergent magnetic field above the surface, and describe an experimental search for this monopolar field using muon spin resonance spectroscopy . Finally, we discuss the implications of an isotropic diagonal magnetoelectric response, and propose candidate materials for such behavior.
 Search for the Magnetic Monopole at a Magnetoelectric Surface, Q. N. Meier et al., Phys. Rev. X 9, 011011 (2019)
9:30 AM - EL03.04.04
Structure and Properties of Freestanding Two-Dimensional Oxide Perovskites
Xiaoqing Pan2,Dianxiang Ji1,Songhua Cai1,Haoying Sun1,Yi Zhang2,Wenpei Gao2,Huaixun Huyan2,Lu Han1,Zhengbin Gu1,Tula Paudel3,Evgeny Tsymbal3,Peng Wang1,Yuefeng Nie1
Nanjing University1,University of California2,University of Nebraska–Lincoln3Show Abstract
Two-dimensional (2D) materials such as graphene and transitionmetal dichalcogenides reveal the electronic phases that emerge when a bulk crystal is reduced to a monolayer. Transition-metal oxide perovskites host a variety of correlated electronic phases, so similar behavior in monolayer materials based on transition metal oxide perovskites would open the door to a rich spectrum of exotic 2D correlated phases that have not yet been explored. Here we report the fabrication of freestanding perovskite films with high crystalline quality almost down to a single unit cell. Using a method based on water-soluble Sr3Al2O6as the sacrificial buffer layer1, recently developed at Stanford University, we synthesize freestanding SrTiO3and BiFeO3ultrathin films by reactive molecular beam epitaxy and transfer them to diverse substrates, in particular crystalline silicon wafers and holey carbon films. We find that freestanding BiFeO3films exhibit unexpected and giant tetragonality and polarization when approaching the 2D limit. Our results demonstrate the absence of a critical thickness for stabilizing the crystalline order in the freestanding ultrathin oxide films. Furthermore, the systematic characterization of the cross-sectional samples by atomic resolution electron microscopy reveals that the crystal symmetry and physical properties such as local electrical polarization are strongly dependent on the local strain and boundary conditions of the film. The ability to synthesize and transfer crystalline freestanding perovskite films without any thickness limitation onto any desired substrate creates opportunities for research into 2D correlated phases and interfacial phenomena that have not previously been technically possible.
10:30 AM - EL03.04.05
Detection of magnetically labeled cells using magnetoelectric magnetic field sensors, Christine Selhuber Show Abstract
11:00 AM - EL03.04.06
Creating the Next Device for Moore’s Law with Room Temperature Quantum Materials
Kepler Computing1Show Abstract
The nanoscale transistor is perhaps the most numerous man made object, exceeding 1018 transistors used in ubiquitous computing and communications devices. However, as we reach the hyper scaled dimensions for electronic transistors (smallest transistors reaching sub 10 nanometer dimension)[i], a search for identifying the next scalable transistor is ongoing. For use in ubiquitous computing, such a “transistor” not only needs able to operate at room temperature but also possess features commensurate with beneficial miniaturization (Moore’s law). We have studied >25 device topologies for new transistor technologies and have considered the use of nearly all the breakthroughs in materials science from the last 3 decades[ii]. We have come to the understanding that new materials and phenomenon enabled by quantum materials form the path to the next “transistor” that is suitable for consumer electronics and cloud computing.
The Technology Need: We describe the imminent need for a revolutionary new transistor for classical Boolean computing based on a) The thermal power limit of the computers reaching the historic trigger point of 10 W/cm2 (Figure 1), this has earlier led the conversion of computing from Bipolar to CMOS in 1980s. Another such trigger is imminent b) The exponential growth in energy demands due to proliferation of compute devices c) The continued need for classic computations that are described by a large variety of computational algorithms (e.g Geometric, combinatorial problems, graphical processing, computational fluid dynamics, prediction of complex physical/biological phenomenon).
A Quantum Materials pathway for new computing[iii]: We will describe a fundamentally new scaling path for computing where we bridge the breakthroughs in quantum materials for creating the next general purpose, room temperature computing technology. The term Quantum Materials is used to describe a broad class of materials that exhibit strong interactions amongst the charge, spin, orbital and lattice degrees of freedom. Over the past 2-3 decades, since the advent of high temperature superconductivity in cuprates, there have been several classes of quantum materials that include i) the CMR manganites where new states of matter and exquisite tunability of such states with external stimuli are driven by the strong electron-electron correlations and the consequent mesoscale phase coexistence, and ii) topological insulators that are driven by strong spin-orbit coupling leading to unusual band topology and Dirac-like fermion behavior, as key examples.
Magneto-electrics and Topological Conversion Path way for Computing[iv] : I will describe the concept device (named Magneto-electric Spin Orbit Logic) to drive high functionality materials in magneto-electrics and topological materials. In particular, the path to computing at aJ/bit (~30X more energy efficient than advanced CMOS) with 10-20X relaxation of the interconnect requirements will be described.
[i] Kuhn, K.J., ….Manipatruni, S., Nikonov, D., Pawashe, C. and Radosavljevic, M., 2012, December. The ultimate CMOS device and beyond. In 2012 International Electron Devices Meeting (pp. 8-1). IEEE.
[ii] Nikonov, D.E. and Young, I.A., 2015. Benchmarking of beyond-CMOS exploratory devices for logic integrated circuits. IEEE Journal on Exploratory Solid-State Computational Devices and Circuits, 1,.
[iii] Manipatruni, S., Nikonov, D.E. and Young, I.A., 2018. Beyond CMOS computing with spin and polarization. Nature Physics, 14(4), p.338.
[iv] Manipatruni, S., Nikonov, D.E., Lin, C.C., Gosavi, T.A., Liu, H., Prasad, B., Huang, Y.L., Bonturim, E., Ramesh, R. and Young, I.A., 2019. Scalable energy-efficient magnetoelectric spin–orbit logic. Nature, 565(7737), p.35.
11:30 AM - EL03.04.07
Stabilization of a New Antiferroelectric Phase of BiFeO3 through Electrostatic Engineering in Oxide Heterostructures
Bastien Grosso1,Quintin Meier1,Nicola Spaldin1
ETH Zürich1Show Abstract
BiFeO3 (BFO) is one of the most studied multiferroic materials because of the coexistence of magnetic and polar orders at room temperature. Here we show that previously unidentified structural phases of BFO, with functional properties different from those of the rhombohedral ferroelectric bulk structure, can be stabilized by exploiting the electrostatic boundary conditions in thin film heterostructures. This provides a complementary approach to the earlier successes in stabilizing some of the many low-energy phases that have been identified computationally, by using coherent heteroepitaxial strain [1,2]. Using density functional theory, we identify a new antipolar phase of BFO and find that the energy barrier to convert it into a ferroelectric phase is small enough for it to be a candidate antiferroelectric. According to our strain calculations and a simple electrostatic model, this antipolar phase can be stabilized with insulating non-polar electrodes for a certain thickness range of the BFO layer on a substrate imposing a small amount of compressive strain; the rhombohedral phase can be recovered by increasing the thickness. These predictions are consistent with a new antipolar phase recently observed experimentally in La1-xBixFeO3/BiFeO3 superlattices, which reveal a double hysteresis loop, characteristic of an antiferroelectric material . Finally, we identify other new low-energy phases for BFO and propose possible ways to stabilize them experimentally.
 O. Diéguez et al., Physical Review B, 83, 094105 (2011)
 H. Béa et al, Physical Review Letters, 102, 217603 (2009)
 J. Mundy et al. arXiv:1812.09615
11:45 AM - EL03.04.08
Understanding Magnetoelectric Switching in Lanthanum-Doped BiFeO3 Thin Films
Yen-Lin Huang1,Rajesh Chopdekar2,Chirs Addiego3,Xiaoqing Pan3,Heng-Jui Liu4,Ying-Hao Chu5,Ramamoorthy Ramesh1
University of California, Berkeley1,Lawrence Berkeley National Laboratory2,University of California, Irvine3,National Chung Hsing University4,National Chiao Tung University5Show Abstract
The key to integrating the concepts of spintronics into conventional nanoelectronics lies with the ability to control the magnetic order in nanoscale devices. With the continuous shrinkage of integrated circuits, the energy efficiency required to control these tiny magnets as power dissipation becomes a determining factor below 7 nm node. Over the past decades, the oxide community has been exploring the materials that can provide opportunities to control magnetism. Among the large investigated materials, multiferroics might be one of the most promising material family. Multiferroics are defined as the materials which possess at least two order of parameters, particularly, the coexistence of ferroelectricity (P) and magnetism (M), and exhibit coupling from one to another. In this talk, I will discuss the magnetoelectric switching mechanism in lanthanum-doped BiFeO3 thin films. BiFeO3 is by far the best-studied multiferroic, which shows strong ferroelectricity (~100 ��C/cm2) and G-type antiferromagnetism, above room temperature. It also shows weak ferromagnetism (MC) induced by the canted spin configuration described by the Dzyaloshinskii–Moriya interaction (DMI). Moreover, these ferroic orderings, P and MC, are strongly coupled, thus one can switch the magnetism by an electric field. However, the strong spontaneous polarization in BiFeO3 needs a large voltage to switch. Here, we introduce the chemical doping to modify the order parameters in BiFeO3 and achieve an ultralow-voltage (< 500 mV) and non-volatile manipulation of ferromagnetism at room temperature. Moreover, while the lanthanum-doping increased, we observed a very different magnetoelectric switching pathway and magnetic anisotropy compare to pure BFO. This discovery leads to the enhancement of perpendicular magnetic anisotropy (PMA) on multiferroics thin film, which will be very attractive to the practical applications. Finally, I will conclude this talk with a summary of current challenges and future direction of multiferroics, especially BFO, toward the low-power electronics.
EL03.05: Magnetoelectrics II
Tuesday PM, December 03, 2019
Hynes, Level 1, Room 101
1:30 PM - *EL03.05.01
Multiferroic Self-Assembled Oxide Nanocomposites Incorporating BiFeO3, YFeO3 and SrFe1-xCoxO3
Caroline Ross1,Shuai Ning1
Massachusetts Institute of Technology1Show Abstract
Self-assembled two phase epitaxial oxide nanocomposites, in which a magnetic phase and a ferroelectric phase are coupled via strain transfer at their interfaces, can exhibit multiferroic and magnetoelectric responses. Such nanocomposites hold promise for making new types of electrically-switchable magnetic devices. The most commonly studied nanocomposite consists of a perovskite matrix (e.g. BiFeO3 (BFO)) surrounding vertical pillars of a ferrimagnetic spinel (e.g. CoFe2O4 (CFO)). An electric field applied to the BFO changes its strain state and hence the strain state and magnetic anisotropy of the CFO, promoting changes in magnetization and even reversal. We will first describe BFO/CFO nanocomposites including strategies for templating the pillar positions and the behavior of (110)-oriented nanocomposites with fin-shaped CFO exhibiting in-plane anisotropy, and compare the structure and properties of nanocomposites grown by sputtering vs. pulsed laser deposition. We then describe nanocomposites containing YFeO3 (YFO) as the ferroelectric phase. Bulk YFO is not ferroelectric, but thin films of YFO grown on certain substrates exhibit a polarization that can exceed 100 µC/cm2. Based on first principles calculations the polarization is attributed to epitaxial mismatch strain which promotes off-centering of the cations. YFO/CFO nanocomposites grown on SrTiO3 (001) substrates show a magnetoelectric coupling in which the ferroelectric hysteresis is sensitive to an in-plane magnetic field. We also demonstrate the control of the magnetic properties of nanocomposites containing SrFe1-xCoxO3 (SFCO) using ionic liquid gating. Single phase films of SFCO are non-magnetic as grown and form either a perovskite or brownmillerite phase depending on deposition conditions and Fe:Co ratio. However, negative gating inserts oxygen and leads to a magnetization of up to 100 emu cm-3 and a structural change from brownmillerite to perovskite with an associated substantial volume change. This magnetic switching is reversible over multiple cycles and is also observed in nanocomposites of SrFeCoO3 codeposited with a spinel phase including Co3O4 and CFO. The inclusion of new materials, SFCO or YFO, in nanocomposites therefore expands the palette of possible structures, properties and control strategies, enhancing the functionality of these magnetoelectric heterostructures.
2:00 PM - *EL03.05.02
A Route to Low Noise Magnetoelectric Sensors—Controlling Magnetic Domain and Domain Wall Effects in Magnetoelectric Sensor Devices
Kiel University1Show Abstract
The role of magnetic domain formation and reorientation processes reveals fascinating physics and is of great relevance for technological applications. Especially the class of magnetic sensors that depend on magnetic thin film technology, rely on magnetic domain control for proper operation. Recent advances in thin film magnetoelectric (ME) composites offer a promising route for sensing ultra-low magnetic signals. Yet, one obstacle of achieving very low limit of detection is caused by magnetic domain activity, which is a well-known noise source in various magnetic field sensing applications. Irreversible and hysteretic magnetization changes from domain nucleation and other hysteretic domain effects impact the sensor’s performance. Moreover, the characteristics of magnetic domains reflect stress induced spatial alterations in the magnetic anisotropy distribution. Overall, due to the formation of magnetic domains in the piezomagnetic phase, the magnetization reversal in magnetic layers is complex.
The role and relevance of magnetic domains and domain walls for the ME response will be discussed in detail. Domain effects in different types of ME devices, including magnetically and electrically modulated thin film devices as well as surface acoustic wave (SAW) devices will be discussed. Domain activity in operating devices is studied from low frequencies, in the hundred kHz range, and at 150 MHz. Domain investigations at the operational frequencies of modulated and SAW sensors are perfomred by time-resolved magneto-optical Kerr effect microscopy.
A direct connection between specific magnetic domain activities and the exhibited noise characteristics is obtained. Even minimal domain activity is restricting magnetic sensor performance. Magnetic noise density and not sensitivity is the main figure-of-merit for optimizing sensor performance. Controlling magnetic domain behavior is a key to improved sensor performance.
Support through the DFG through the Collaborative Research Centre SFB 1261 is highly acknowledged.
1. N. O. Urs, V. Röbisch, S. Toxværd, S. Deldar, R. Knöchel, M. Höft, E.Quandt, D. Meyners, J. McCord, Direct linking specific magnetic domain activities and magnetic noise in modulated magnetoelectric sensors (submitted)
2. M. Jovičević Klug, L. Thormählen, V. Röbisch, S. Salzer, M. Höft, E. Quandt D. Meyners, J. McCord, Applied Physics Letters 114, 192410 (2019)
3. R.B. Holländer, C. Müller, J. Schmalz, M. Gerken, J. McCord, Scientific Reports 8, 13871 (2018)
4. A. Kittmann, P. Durdaut, S. Zabel, J. Reermann, J. Schmalz, B. Spetzler, D. Meyners, N.X. Sun, J. McCord, M. Gerken, G. Schmidt, M. Höft, R. Knöchel, F. Faupel, E. Quandt, Scientific Reports 8, 278 (2018)
5. S. Salzer, V. Röbisch, M. Klug, P. Durdaut, J. McCord, D. Meyners, J. Reermann, M. Höft, R. Knöchel, IEEE Sensors Journal, PP, 99 (2017)
6. V. Röbisch, S. Salzer, N. Urs, J. Reermann, E. Yarar, A. Piorra, C. Kirchhof, E. Lage, M. Höft, G. Schmidt, R. Knöchel, J. McCord, E. Quandt, D. Meyners, Journal of Materials Research 1-11 (2017)
7. N.O. Urs, B. Mozooni, P. Mazalski, M. Kustov, P. Hayes, S. Deldar, E. Quandt, J. McCord, AIP Advances 6, 055605 (2016)
8. J. McCord, Journal of Physics D: Applied Physics 48, 333001 (2015)
9. N. O. Urs, I. Teliban, A. Piorra, R. Knöchel, E. Quandt, J. McCord, Applied Physics Letters 105, 202406 (2014)
10. E. Lage, N. O. Urs, V. Röbisch, I. Teliban, R. Knöchel, D. Meyners, J. McCord, E. Quandt, Applied Physics Letters 104, 132405 (2014)
2:30 PM - *EL03.05.03
Understanding the Magneto-Mechanical Response of Terfenol-D Micro/Nano-Structures
Joseph Schneider1,Mohanchandra Panduranga1,Zhuyun Xiao1,Taehwan Lee1,Christoph Klewe2,Rajesh Chopdekar2,Padraiiac Shafer2,Alpha N'Diaye2,Elke Arenholz2,Rob Candler1,3,Gregory Carman1
University of California, Los Angeles1,Lawrence Berkeley National Laboratory2,California Nanosystems Institute3Show Abstract
The field of nanoscale strain mediated multiferroics has grown considerably during the last decade due to the promise offered for efficiently controlling magnetism in the small scale. Strain mediated multiferroics consist of piezoelectrics mechanically coupled to magnetoelastic materials. An applied voltage to the piezoelectric induces a strain in the magnetoelastic material reorienting the magnetic spin moments. This approach is contrasted with electrical current approaches to control magnetic moment such as to reorient small magnetic bits with spin transfer torque STT. For informational purposes the energy required to reorient a 100 nm magnetic memory bit using STT is on the order of 100 fJ with the promise that strain mediated multiferroic is less than 0.1 fJ, i.e. > 4 orders of magnitude improvement. While strain mediated multiferroic approaches promise substantial efficiency improvements, many research effoerts focus on magnetic materials that are on moderately or weakly magnetoelastic due to fabrication related issues. In this presentation a review of progress on fabricating and testing Terfenol-D (Tb0.3Dy0.7 Fe1.92) small scale structures, i.e. one of the highest room temperature magnetoelastic materials, is described to help advance the multiferroic field. This work includes discussions of fabrication, magnetic spin assessment, thermal effects, corrosion properties, and application demonstrated work.
Polycrystalline Terfenol-D thin films (<100 nm) are produced using a DC magnetron sputtering process on Sapphire, Si and PMN-PT substrates. The crystallized Terfenol-D films are micropatterned with photolithographic methods using Ar etching. The continuous and micropatterned (<20 microns) structures are characterized with XRD, SQUID, MOKE, MFM, PEEM, and XMCD to evaluate magnetoelastic properties. For micro-patterned structures as large as 20 microns in diameter, magnetic single domain structures are observed (MFM and PEEM) which is unusually large for this soft magnetic material. The large single domain behavior is attributed to the residual stresses produced during fabrication to further stabilize the magnetic spin states along preferred magnetic easy axis. Furthermore, an absence of oxidation is observed in these small-scale structures. While there is a capping layer on the Terfenol-D films, one would expect stress corrosion cracking to arise along the micropatterned side walls but this is absent. We attribute the corrosion absence to both the capping layer as well as the residual stresses preventing stress propagation and arresting oxidation. XMCD results on elemental spin states in the Terfenol-D reveal that the magnetic moments predominantly arise from the Tb and Dy spin/orital contributions with Fe magnetic spin pointing in the opposite direction, i.e. ferrimagnetic material. However, the main contribution for the Dy element arises from orbital moment rather than spin which is slightly unusual. Furthermore, the Dy elements spin orbital moment changes prominently as a function of temperature. We believe that the spin orbit moment coupling arising from Dy significantly contributes to the changes observed in the magnetocrystalline anisotropy as a function of temperature. Finally, demonstrations of a multiferroic PMN-PT/Terfenol-D (20 micron size microstructure) to capture and release magnetic particles attached to cells are presented for showing efficient control of magnetism in the small scale.
3:30 PM - *EL03.05.04
Materials for STT-MRAM Applications
Virat Mehta1,Guohan Hu1
IBM T.J. Watson Research Ctr1Show Abstract
Spin Transfer Torque Magnetic Random Access Memory (STT-MRAM) is a type of emerging memory which holds the promise of high speed, high endurance, non-volatility, and good scalability. Since the theoretical prediction of the STT switching mechanism in 1996, significant progress has been made in the field, largely through materials innovations. In this talk, I will review the key materials discoveries that enabled the advancement of STT-MRAM technology. This includes the theoretical prediction and experimental realization of large tunneling magneto-resistance (TMR) with MgO tunnel barrier and the discovery of CoFeB based materials with interfacial perpendicular magnetic anisotropy (iPMA). This talk will also discuss our recent results at IBM on methods to lower the switching current of Spin-Transfer-Torque MRAM and achieve low write-error-rate by using optimized magnetic materials.
4:00 PM - EL03.05.05
Efficient Energy Harvesting from Low Ambient Stray Magnetic Field Using Magnetoelectric Coupled Magneto-Mechano-Electric Generator
Min Gyu Kang1,Hyeon Lee2,RamMohan SriRamdas1,Shashank Priya1
Pennsylvania State University1,Virginia Tech2Show Abstract
Smart infrastructure functionalized with Internet of Things (IoT) technology is driving need of the wireless sensor network system and its sustainable power source. Magneto-mechano-electric (MME) energy conversion is the most promising technology to supply a sustainable power into the IoT sensor devices as it efficiently converts low frequency stray magnetic field (50/60 Hz), which exists everywhere in modern infrastructure, into the electricity. However, currently reported MME generators produce relatively low power under low magnetic field (≤300 μT), which commonly exist in infrastructure. In this work, we demonstrate magnetoelectric (ME) coupled MME generator to produce high output power from low amplitude magnetic field. Comprehensive energy conversion mechanisms of ME coupled MME generator, including structural factors and contribution of ME coupling on power output, are investigated in order to achieve high energy conversion efficiency in low amplitude magnetic field. Building upon the mechanism study, an optimum MME generator, producing milliwatt power below 300 μT magnetic field, is realized utilizing outstanding magnetoelectric composite cantilever. Exploiting the harvested power near a home appliance, sustainable powering integrated sensors and wireless communication system is demonstrated. The fundamental study performed in this work provides a direction to achieve the efficient magnetic field energy harvesting and this will enable practical implantation of the IoT devices into the smart infrastructure.
4:15 PM - EL03.05.06
Electrically Modulated Magnetoelectric Thin-Film Sensors for Sensing Small Magnetic Fields
Patrick Hayes1,Sebastian Toxværd1,Phillip Durdaut1,Matic Jovičević Klug1,Dmitri A. Burdin2,Viktor Schell1,Yuri K. Fetisov2,Reinhard Knöchel1,Jeffrey McCord1,Eckhard Quandt1
Kiel University1,MIREA - Russian Technological University (MIREA)2Show Abstract
Magnetoelectric (ME) thin film composites consisting of a sputtered piezoelectric (PE) and a magnetostrictive (MS) layer may be employed for measurements of magnetic fields passively, i.e. an AC magnetic field generates an ME voltage by mechanical coupling of the MS deformation to the PE phase, thus exploiting the direct ME effect. In order to achieve high field sensitivities a magnetic bias field, necessary to operate at the maximum piezomagnetic coefficient of the MS phase is used, using mechanical resonances further enhances this direct ME effect size. Despite being able to detect very small field amplitudes passively, by exploiting mechanical resonances, implies a limitation to available signal bandwidth, because of rather high Q factors. The requirement for a magnetic bias field along with the inability to detect DC magnetic fields makes practical implementation troublesome.
In the presented work the PE phase of such thin film ME composites is actively excited, thus exploiting the converse ME effect , remedying shortcomings of the direct ME effect. The experimental work makes use of surface micromachined thin film cantilever composites of mesoscopic scale (25mm x 2.5mm x 0.35 mm) of which a high frequency mechanical resonance at about 500 kHz, showing a mechanical quality factor of about Q~1000 is analyzed. This mechanical oscillation, being rigidly coupled to the magnetostrictive material, leads to a voltage induced in a pickup coil surrounding the sensor composite, giving rise to magnetoelastic interactions. Major signal components of bio magnetism lie in the range from DC to 500 Hz and amplitudes are of vanishingly small amplitude < ~ 50 pT, this regime is targeted by this research. This entirely passive readout, combined with low spatial and power requirements makes the presented ME sensor system suitable for integration into arrays as anticipated for biomagnetic imaging. The converse ME voltage response with respect to small external fields shows sensitivities up to 40 kV/T, offering linearity up to a field magnitude of several μT, no external magnetic driving field is required. The sensor sensitivity scales nearly linearly with drive amplitude supplied to the PE phase, unfortunately the measured noise floor in the frequency regime of interest shows an abrupt increase as soon as an excitation threshold of about 200 mV is reached. Massive magnetization activity in the MS phase is presumably the dominant source of noise. High speed vibrometry measurements give insight concerning the high frequency mechanical oscillation mode, magneto optical imaging reveals magnetoelastic modulations of the MS phase.
Furthermore, we demonstrate the performance of electrically modulated thin film ME composites, using magnetron sputtered AlN and amorphous FeCoSiB films. This approach enables composite magnetoelectrics to detect low DC (~ 250 pT/sqrt(Hz)) as well as AC (~ 75 pT/sqrt(Hz) @ 10 Hz) magnetic fields without the need of an external magnetic AC or DC bias field. Finally, lower system noise is achieved using specially tailored antiparallel exchange biased MS layers thus inhibiting domain wall activity and even further improve the detection limit.
Funding via DFG, SFB1261 “Magnetoelectric Sensors: From Composite Materials to Biomagnetic Diagnostics” is gratefully acknowledged.
 Hayes, P., V. Schell, S. Salzer, D. Burdin, E. Yarar, A. Piorra, R. Knöchel, Y. K. Fetisov, and E. Quandt. “Electrically modulated magnetoelectric AlN/FeCoSiB film composites for DC magnetic field sensing.” Journal of Physics D: Applied Physics 51, no. 35 (2018): 354002. doi:10.1088/1361-6463/aad456.
4:30 PM - *EL03.05.07
Voltage Controlled Ferromagnetic Resonance for Magnetic Field Sensing and Beyond
Dominic Labanowski2,Sayeef Salahuddin1
University of California, Berkeley1,Sonera Magnetics2Show Abstract
Magnetostriction makes it possible to drive a magnet into resonance using purely a voltage signal. In a piezoelectric-ferromagnetic bi-layer, an alternating voltage applied to the piezoelectric transforms into a pseudo alternating magnetic field for the magnet. Combined with an internal static field that comes from the magnetic anisotropy, this alternating magnetic field can put the magnet into resonance. We shall describe our recent experimental work that demonstrates this effect in a LiNbO3/Ni heterostructure. It was observed that a highly efficient transduction (>99.9%) is possible in this process. A magnet put into resonance in this way also shows potential for sensing very small magnetic fields (~pT/sqrt(Hz)). In addition, they can be used for locally driving two level quantum systems without needing an optical excitation. We shall discuss our recent progress regarding these applications.
EL03.06: Poster Session II: Ferroelectrics and Metal-Insulator Transition
Tuesday PM, December 03, 2019
Hynes, Level 1, Hall B
8:00 PM - EL03.06.01
Some Interesting Properties Associated to an Unusual High Iron Valence in the FeSr2YCu2O7.85 Superconducting Cuprate
Miguel Angel Alario-Franco1,Sara Lopez-Paz1,Xabier Martinez de Irujo-Labalde1,Jorge Sanchez-Marcos1,Clemens Ritter1,Emilio Moran1
Universidad Complutense1Show Abstract
Iron containing perovskites have been intensively studied as potential functional materials with applications ranging from Solid Oxide Fuel Cell (SOFC) cathodes and magnetoelectric multiferroics to half-metallic magnetoresistive materials. On the other hand, high temperature superconducting cuprates are another example of correlated materials that are placed in the frontier between localized and itinerant electronic behaviour, with superconductivity emerging from a Mott insulating type material upon doping.
The title material combines two functionalities: magnetism and superconductivity, associated to the presence of separated Fe-O2 and Cu-O2 layers orderly stacked along the c-axis
The formal presence of FeV cations resulted from ozone oxidation, leads to a long-range magnetic ordering, coexisting with the superconducting interactions (TN= 110 K > Tc= 70 K). The somewhat unexpected A-type AFM structure, with a μ(Fe) approximately 2 μB magnetic saturation moment, associated to the hypervalent iron sublattice, suggests an unusual low spin state for the iron cations; on the othe hand, the low dimensionality of the magnetic structure results in a soft switching towards ferromagnetism under small external magnetic fields.
It is also interesting to mention the relatively high superconducting Tc in a highly overdoped cuprate 
The role of the crystal structure and the high charge concentration in the stabilization of this unusual electronic configuration for the iron cations is discussed.
 X. Martínez de Irujo-Labalde, D. Muñoz-Gil, E. Urones-Garrote, D. Ávila-Brande, S. García-Martín, J. Mater. Chem. A 2016, 4, 10241– 10247.
 N. A. Spaldin, R. Ramesh, Nat. Mater. 2019, 18, 203–212.
 T. K. Mandal, M. Greenblatt, in Funct. Oxides, John Wiley & Sons, Ltd, Chichester, UK, 2010, pp. 257–293.
 M. Imada, A. Fujimori, Y. Tokura, Rev. Mod. Phys. 1998, 70, 1039– 1263
 A. Gauzzi, Y. Klein, M. Nisula, M. Karppinen, P. K. Biswas, H. Saadaoui, E. Morenzoni, P. Manuel, D. Khalyavin, M. Marezio, and T. H. Geballe
8:00 PM - EL03.06.02
Engineering Electronic Coupling of Metal-Insulator Phases at SmNiO3/NdNiO3 Interfaces
Claribel Dominguez1,Marta Gibert2,Jennifer Fowlie1,Alexandru Bogdan Georgescu3,Yajun Zhang4,Alain Mercy4,Bernat Mundet1,5,Duncan Alexander5,Philippe Ghosez4,Andrew Millis3,Antoine Georges3,Jean-Marc Triscone1
University of Geneva1,University of Zurich2,Flatiron Institute3,University of Liège4,École Polytechnique Fédérale de Lausanne (EPFL)5Show Abstract
Perovskite rare earth nickelates (RNiO3), where R is a rare earth cation are well-known for the sharp metal-to-insulator transition (MIT) observed when decreasing temperature, at T = TMI (R different than La) (1-3). Many studies have focused on manipulating the MIT for instance through strain (4), growth direction (5) and superlattice heterostructure (6). In this work, we use experimental and theoretical methods to design and study superlattices of two distinct rare earth nickelate oxides SmNiO3 (SNO) and NdNiO3 (NNO) that in bulk form show a MIT at two very different temperatures (400K and 200K, respectively). We find that these new complex oxide superlattices display different behavior than that of either bulk material, showing either a single MIT at an intermediate temperature, or two transition temperatures that converge asymptotically towards the strained bulk values of each material. This system allows the origin of the coupling at such interfaces to be studied. We show that the length scale of the MIT transition in the superlattices is set not by the length scale of the propagation of structural motifs across the two materials, which ab-initio calculations and TEM analysis suggest is minimal, but rather by the balance between the energy cost of having metallic-insulating domain walls (the cost of bending the order parameter across the metallic-insulating interface) and the energy gain of the bulk phases.
1. M. L. Medarde, Structural, magnetic and electronic properties of RNiO3 perovskites (R = rare earth), Journal of Physics Condensed Matter, 9, 1679 (1997).
2. G. Catalan, Progress in perovskite nickelate research, Phase Transitions 81 729-749 (2008).
3. S. Catalano, et al., Rare-Earth Nickelates RNiO3: Thin films and heterostructures, Rep. Prog. Phys. (2017).
4. S. Catalano, et al., Electronic transitions in strained SmNiO3 thin films, APL Materials 2 116110 (2014).
5. S. Catalano, et al., Tailoring the electronic transitions of NdNiO3 films through (111)pc oriented interfaces, APL Materials 3 062506 (2015).
6. Z. Liao, et al., Metal-insulator-transition engineering by modulation tilt-control in perovskite nickelates for room temperature optical switching, Proc. Natl. Acad. Sci. 115 (2018).
8:00 PM - EL03.06.03
Length Scales and Heterostructuring in the Metal-Insulator Transition of RNiO3
Alexandru Bogdan Georgescu1,Claribel Dominguez2,Oleg E. Peil3,Jennifer Fowlie2,Ankit S Disa4,Jean-Marc Triscone2,Antoine Georges1,2,5,Andrew Millis1,6
Flatiron Institute1,University of Geneva2,Materials Center Leoben3,Max Planck Institute for Solid State Research4,College de France5,Columbia University6Show Abstract
The metal-insulator transition (MIT) of transition metal oxides is often associated with a simultaneous lattice and electronic symmetry breaking; however the relative roles of the electronic and lattice degrees of freedom is still an unresolved question. Further, the length-scale of the metal-insulator transition and what sets it is not well understood. Through the study of heterostructures of rare-earth nickelates (RNiO3), we get insight into these questions. First, using a combination of first-principles, many-body computational methods and experiment [1,2,3,4], we study the effect of heterostructuring NdNiO3 with the band insulator NdAlO3. We find two competing effects: the effective lattice cost to disproportionate the NiO6 octahedra increases due to resistance from the interfacial Al-O bonds. Separately, electronic confinement favors an insulating state by lowering the electronic kinetic energy. These effects combined lead to a higher MIT temperature than the bulk, accompanied by a lower signature of bulk disproportionation on the X-Ray spectra. To understand the length scales involved in the MIT we study superlattices of two nickelate materials that have the same type of transition but two different transition temperatures (NdNiO3~150K and SmNiO3~400K). We find that for thin enough layers of each material, a single transition at an intermediate temperature exists, while at higher layer thickness two MITs appear at temperatures that asymptotically tend to the bulk MIT temperatures with increasing layer thickness. We find that this behavior is set not by the gradual propagation of structural motifs, but by the competition between the domain wall energy cost at the interface between the metallic and insulating materials and the bulk free energy cost of the materials not being in their favored state. Our work thus opens new paths in the systematic study of complex oxide materials.
 A. B. Georgescu, O. E. Peil, A. S. Disa, A. Georges and A. J. Millis, in press at PNAS, arXiv:1810.00480
 O. E. Peil et al, in press at PRB, arXiv:1809:03720
 Q. Han and A. J. Millis PRL 121, 067601 (2018), arXiv:1801.06215
 A. Disa, A.B. Georgescu et al PRM 1, 024410 (2017), arXiv:1809.07810
8:00 PM - EL03.06.04
Ferroeletric Polarization-Switching Dynamics and Fatigue Behavior in Si-Doped HfO2
Myeongseop Song1,Seung Chul Chae1
Seoul National University1Show Abstract
HfO2-based ferroelectrics exhibits two regimes of “wake-up” and “fatigue” in which remnant polarization increases and decreases during electric field cycling, respectively. These two phenomena are considered as the effect of defect generation and diffusion including redistribution of oxygen vacancies. The structural transition in the wake-up stage has been focused in ferroelectric HfO2 thin film. However, in order to operate a reliable device, it is necessary to understand the ferroelectric characteristics and dielectric properties in wake-up and fatigue processes.
Grimley et al. proposed that the variation of bulk defect concentration which constrains domain wall motion by defect pinning is the origin of fatigue behavior. However, Lou et al. suggested that the structure decomposition caused by charge carrier injection was the main reason for fatigue endurance. The mechanism of fatigue behavior of HfO2 thin films is still unclear. So, understanding of the ferroelectric characteristics with respect to the fatigue behavior is required for practical device operation.
We report on the ferroelectric switching dynamics of fatigued 4.2% Si-doped HfO2 thin film. Prior to the fatigue behavior, Si-doped HfO2 thin films exhibited the wake-up behavior where the remnant polarization value increased with the repeat of external bias cycling. After the wake-up behavior, Si-doped HfO2 film exhibited the degradation of the remnant polarization value alongside the sweep of external bias, i.e., fatigue behavior. The investigation of ferroelectric switching dynamics revealed the retardation and recovery of the characteristic switching time for ferroelectric nucleation coincident with the wake-up behavior and fatigue behavior, respectively. We analyzed the interface trap density with the capacitance-voltage characteristics and attributed the fatigue behavior to the increase of oxygen vacancies with fatigue behavior.
8:00 PM - EL03.06.05
Unconventional Stability of Sub-Loop Behavior in Ferroelectric HfO2
Kyoungjun Lee1,Seung Chul Chae1
Seoul National University1Show Abstract
Ferroelectricity with partial polarization switching is considered as one of a feasible candidate for an analog device in the form of the ferroelectric tunnel junction and ferroelectric transistor. However, deterministic control of ferroelectric polarization states with conventional ferroelectric materials have been met with accessibility problems due to the complex nature of ferroelectric switching mechanism and/or defect mediated uncertainty. Ferroelectric HfO2 thin film has been investigated intensively as an alternative to perovskite materials in ferroelectric random access memory due to the advantages for nonvolatile memory applications, such as good scalability, compatibility with conventional complementary metal-oxide-semiconductor (CMOS) process technology.
Here, we report unprecedented stability of the sub-loop switching behavior in ferroelectric HfO2. We suggest that the stable accessibility with robust stability of multiple polarization states in ferroelectric HfO2 can be attributed to the large activation field for ferroelectric switching with small critical volume for the ferroelectric nucleation of HfO2. The switching dynamics indicated a large activation field for ferroelectric switching. The temperature dependence of hysteresis and piezoresponse force microscopy measurements indicated a small critical volume for ferroelectric nucleation. The theoretical calculation demonstrated the stable switching energy landscape for single dipole flip in ferroelectric HfO2. Monte-Carlo simulation demonstrated that the small critical volume for nucleation induces stable accessibility of multiple polarization states in ferroelectric HfO2.
8:00 PM - EL03.06.06
Electromechanical Performance of Core-Shell Structured Relaxor Ceramics and the Impact of Interfacial Stress
Julia Glaum1,2,Yooun Heo2,Matias Acosta3,Jan Seidel2,Manuel Hinterstein2,4
Norwegian University of Science and Technology1,UNSW Sydney2,Technische Universität Darmstadt3,Karlsruhe Institute for Technology4Show Abstract
The unique properties displayed by canonical relaxor systems, such as the electric field induced transformation from a pseudo-cubic relaxor state to a polar ferroelectric state, the associated huge strain  and the phase transition mediated polarization reversal mechanism , make these materials highly interesting objects for fundamental studies as well as versatile components for industrial applications.
Especially, the achievement of high strains has drawn significant attention, the origin of which is based on the reversibility of the phase transformation between the ferroelectric and the relaxor state . Many relaxor-ferroelectric systems exhibiting high actuating performance are located in the morphotropic phase region. They often exhibit multiple crystallographic phases arranged as core and shell within single grains and their ability to adapt the phase ratio depending on the external stimuli , is another important factor contributing to their exceptional electromechanical performance.
Here, we report on the development of interfacial stresses between different crystallographic phases in a multiphase (Bi1/2Na1/2)TiO3-BaTiO3 relaxor ceramic as induced by thermal treatment. Upon electric field application, this system exhibits an “intrinsic core-shell structure” of a polar minority phase embedded into a polar majority phase. While the majority phase stays stable with increasing temperature up to the transition into the relaxor state, a gradual de-texturization of the minority phase is observed over the whole temperature range. The surface domain structure was found to decay already at significantly lower temperatures than expected from bulk observations. Development of interfacial stresses due to thermal expansion mismatch between majority and minority phases as well as differences in local stress state between surface and bulk are discussed as driving factors of the phase transition dynamics.
Tailoring of interfacial stresses through adaption of phase fractions opens up a pathway to optimize the strain performance of actuator materials and can become a useful tool for the stabilization of usually metastable crystallographic phases as well as for property tuning e.g. in piezotronics.
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 S.-T. Zhang, A. B. Kounga, E. Aulbach, H. Ehrenberg, J. Rödel, Appl. Phys. Lett. 2007, 91, 112906.
 J. Glaum, H. Simons, J. Hudspeth, M. Acosta, J. E. Daniels, Appl. Phys. Lett. 2015, 107, 232906.
 M. Hinterstein, M. Knapp, M. Hölzel, W. Jo, A. Cervellino, H. Ehrenberg, H. Fuess, J. Appl. Crystallogr. 2010, 43, 1314.
 M. Hinterstein, L. A. Schmitt, M. Hölzel, W. Jo, J. Rödel, H.-J. Kleebe, M. Hoffman, Appl. Phys. Lett. 2015, 106, 222904.
8:00 PM - EL03.06.07
Large Pyroelectric Energy Conversion Density in Lead-Free Relaxor-Ferroelectric Heterostructure
Sangram Pradhan1,Amrit Sharma1,Makhes Behera1,Bo Xiao1,Messaoud Bahoura1
Norfolk State University1Show Abstract
The need for efficient energy utilization is driving research into ways to harvest waste-heat which is ubiquitous, abundant and free. Thermal harvesting is a promising method for capturing freely available heat and converting it to a more usable form, such as electrical energy. Thermal harvesting for low power electronic devices using ferroelectric materials is one of the emerging areas of research because these ferroelectric materials possess spontaneous polarization and exhibit excellent piezoelectric as well as pyroelectric coefficients. These materials are unique as they only sense time-dependent temperature change to generate electric power. We have grown lead-free BaZr0.2Ti0.8O3 (BZT)/ Ba0.7Ca0.3TiO3 (BCT) multilayer heterostructures and studied their structural, dielectric, ferroelectric, and pyroelectric properties. The BZT/BCT multilayer epitaxial heterostructures were grown on SrRuO3 (SRO) buffered SrTiO3 (STO) single crystal substrate by optimized pulsed laser deposition technique. The large angle x-ray scans showed only diffraction peaks from the substrate and pseudocubic reflections (l00) from the multilayer heterostructure, confirming that these films are phase pure, highly crystalline, and epitaxial in nature. The atomic force microscopy (AFM) studies indicate that the surface roughness is low and that film growth is of high quality. The ferroelectric phase transitions have been probed above room temperature with a relaxor behavior. The polarization versus electric field (P-E) measurement shows that the multilayer heterostructure exhibits slim and well-saturated hysteresis loop with high saturation and low remnant polarization of 100 and 20 µC/cm2, respectively at 1.7 MV/cm. Solid-state, thin-film devices, that convert low-grade heat into electrical energy, are demonstrated from temperature dependent P-E loops using pyroelectric Ericsson cycles with energy conversion density of 1.61 J/cm3. Our findings suggest that the BZT/BCT multilayer ferroelectric thin film may be competitive with other thermoelectric materials for low-grade thermal harvesting.
8:00 PM - EL03.06.08
Ferroelectricity in Bi4NbO8Cl Single Crystal Nanosheet
Zhizhong Chen1,Jian Shi1
Rensselaer Polytechnic Institute1Show Abstract
While ferroelectric-field-controlled Rashba-Dresselhaus effect has long been proposed as a method to manipulate the valley and spin degrees of freedom in ferroelectrics with strong spin-orbit coupling, the experimental realization of such device concepts remains limited. Although ferroelectric two-dimensional (2D) materials with strong spin-orbit coupling have been widely investigated, most chalcogenide layered 2D or quasi 2D materials considered suffer from low band gap, low Curie temperature or high electrical leakage, rendering the electrical control difficult at room temperature, while the insulating nature of most ferroelectric (quasi-) 2D oxides with heavy elements limits their optical activity. In this work, we report the first experimental observation of ferroelectricity in a quasi-2D 10~100 nm thick nanosheet Sillen-Aurivillius semiconducting split-ion oxyhalide perovskite at room temperature. Optoelectronic, transport and temperature-dependent time-resolved photoluminescence studies show that Bi4NbO8Cl single crystal exhibits a direct band gap of 2.4 eV, decent optical quantum efficiency and carrier dynamics, making it promising candidate for photon-valley coupling. Electrical transport shows up to 100× I-V rectification in Bi4NbO8Cl single crystal nanosheet-based planar devices with symmetric graphite as electrodes. By electrical poling, the diode polarity becomes switchable, rendering repeatable rectified current. Such diode effect in Bi4NbO8Cl is attributed to the asymmetric Schottky barriers at Bi4NbO8Cl–graphite interfaces that could be adjusted by switchable ferroelectric dipoles. In the oxyhalide Bi4NbO8Cl, the combination of appropriate band gap from ion splitting, considerable visible light optical quantum efficiency, strong polarization and the possible strong spin-orbit coupling from Bi provides a novel design platform for realizing emergent spin-orbitronics.
8:00 PM - EL03.06.09
Local Ferroelectric Properties of Free-Standing Single-Crystal Complex Oxides
Saidur Bakaul1,Amanda Petford-Long1,Claudy Serrao2,Mathew Cherukara1,Sayeef Salahuddin3,Ramamoorthy Ramesh4,Dillon Fong1,Tao Zhou1,Martin Holt1
Argonne National Laboratory1,Intel Corporation2,University of California, Berkeley3,University of California Berkeley4Show Abstract
The last few decades have seen significant scientific discoveries in single crystal complex oxide materials including colossal magnetic resistance, superconductivity, voltage control of magnetism and many different ferroic orders, many of which could lead to completely new applications. However, integration of such oxides using direct synthesis on microelectronics-platforms such as Si, amorphous SiO2, GaN, and unconventional flexible substrates has faced significant challenge due to various growth-related issues and the interface chemistry at high temperature. Therefore, the functionality and performance that are otherwise available for epitaxial, single-crystal, perovskite materials have remained unachievable in microelectronic devices for a long time. The recent invention of complex oxide layer transfer techniques (LTT) has opened a promising route to the monolithic integration of these materials with arbitrary substrates ,,,– thus offering a possible replacement to the rarely-successful direct growth techniques.
In LTT, complex oxides epitaxially grown on the lattice-matched substrate are made free-standing and then interfaced with arbitrary material on-demand. Although proof-of-concept devices such as field effect transistor and memory devices have already been demonstrated using such transferred complex oxide ferroelectric (FE) materials,[1,2] little is known about their ferroic properties, particularly at the mesoscopic length scale. In this work, we have studied free-standing, single-crystal PbZr0.2Ti0.8O3 using piezoforce (PFM) and electrostatic force microscopy (EFM) and synchrotron X-ray nanodiffraction techniques. We find that the epitaxial strain imposed on the ferroelectric layers by the substrate during growth by pulsed laser deposition technique is alleviated when the layers are made free-standing. The reduction of elastic strain slightly widens the domain walls, reduces the spontaneous polarization and increases the piezoelectric response. We have studied ferroelectric properties of both the top layers and interfacial layers (which were in contact with the substrate) and found a negligible difference between them. This hints that the intrinsic dead-layer issues may not be the limiting factors for utilizing transferred epitaxial layers in electrostatically controlled devices.
 S. R. Bakaul, C. R. Serrao, O. Lee, Z. Lu, A. Yadav, C. Carraro, R. Maboudian, R. Ramesh, S. Salahuddin, Adv. Mater. 2017, 29, 1605699.
 S. R. Bakaul, C. R. Serrao, M. Lee, C. W. Yeung, A. Sarker, S. L. Hsu, A. K. Yadav, L. Dedon, L. You, A. I. Khan, J. D. Clarkson, C. Hu, R. Ramesh, S. Salahuddin, Nat. Commun. 2016, 7, 10547.
 D. Lu, D. J. Baek, S. S. Hong, L. F. Kourkoutis, Y. Hikita, H. Y. Hwang, Nat. Mater. 2016, 15, 1255.
 L. Shen, L. Wu, Q. Sheng, C. Ma, Y. Zhang, L. Lu, J. Ma, J. Ma, J. Bian, Y. Yang, A. Chen, X. Lu, M. Liu, H. Wang, C. L. Jia, Adv. Mater. 2017, 29, 1702411.
8:00 PM - EL03.06.10
Novel Epitaxial Strain Effects on the Hybrid Improper Ferroelectrics from First-Principles
Xuezeng Lu1,James Rondinelli1
Northwestern University1Show Abstract
Epitaxial strain is a powerful tool to generate ferroelectricity owing to polarization-strain coupling. Local lattice degrees-of-freedom such as rotations of metal-oxygen octahedral also couple to strain, and can be used to tune a material’s oxygen rotational-related properties such as metal-insulator transitions and magnetic reconstruction by strain. Here, we first use electronic structure calculations to investigate the strain effects on (001) thin films of the hybrid-improper ferroelectric (HIF) A3B2O7 compounds. Surprisingly, other than the bulk polar Cmc21 phase, we find a new nonpolar phase becomes the ground state under both experimentally accessible biaxial compressive and tensile strains, which is beyond the people’s believe about the rule of the polarization-strain coupling. Furthermore, the generality of the polar-to-nonpolar (N-NP) transition in HIFs (not only in A3B2O7 compounds) leads us to find a novel route to tune the physical properties that are classified as mechanical, optical and magnetic responses, which we also propose could be electric-field tunable, near the P-NP phase transition boundary. Our results may offer a route to search for new functionalities in hybrid-improper ferroelectrics.
8:00 PM - EL03.06.11
Pure Piezoelectricity Generation by a Flexible Nanogenerator Based on Lead Zirconate Titanate Nanofibers
Yongsok Seo1,Horim Lee1,Hoyeon Kim1
Seoul National University1Show Abstract
Lead Zirconate Titanate (PbZr0.52Ti0.48O3, PZT) alloy has been extensibly studied to be used for piezoelectric nanogenerators to harvest energy from mechanical motions. In this study, PZT nanofiber-based nanogenerators were fabricated to test its true piezoelectric performance without triboelectric effect. Aligned PZT nanofibers were fabricated by sol-gel electrospinning process. The thickness, area, and orientation of the PZT textile made by electrospinning the PZT solution onto multi-pair metal wires or metal mesh were controlled to form a composite textile. After the calcination, the PZT textile mixed with polydimethylsiloxane (PDMS) was placed between two flexible ITO-PEN substrates. The performance parameters of the nanogenerators were investigated under the bending motion, which excludes the triboelectric effect. The assembled nanogenerator of an area of 8 cm2 and a thickness of 80 mm could generate an electrical output voltage of 1.1 V and a current of 1.4 mA under the bending strain. The piezoelectric voltage depended on the thickness of the PZT textile, while the piezoelectric current depended on both the thickness and the area of the PZT textile. The electrical performance of the device was significantly affected by the orientation of the PZT fiber and the bending direction. The output voltage and the output current were strain-dependent, while the total integrated charge was independent of the strain rate. The properties of the flexible nanogenerator could be quantified to verify the pure piezoelectric performance of the device.
8:00 PM - EL03.06.12
Polymorphic Phase Transition in BaTiO3 by Ni Doping
Nguyen Xuan Duong1,Jong-Seong Bae2,Jongchul Jeon3,So Yeon Lim4,Soo Han Oh5,Aman Ullah1,Muhammad Sheeraz1,Jin San Choi1,Jae-Hyeon Ko5,Sang Mo Yang4,Kyou-Hyun Kim3,Ill Won Kim1,Chang Won Ahn1,Tae Heon Kim1
University of Ulsan1,Korea Basic Science Institute (KBSI)2,Korea Institute of Industrial Technology3,Sookmyung Women’s University4,Hallym University5Show Abstract
Hexagonal barium titanate (h-BaTiO3, P63/mmc), which is structurally non-perovskite and energetically stable above 1460 °C, can be an excellent platform for designing an exotic phase which does not exist in nature and for achieving new room-temperature multiferroics with high performance. Owing to the high synthetic temperature, a phase transition to the h-BaTiO3 and the related physical properties have not been studied in detail. In this work, we experimentally demonstrate a structural phase transition from perovskite BaTiO3 with tetragonal symmetry to non-perovskite hexagonal polymorph in Ni-doped BaTiO3 ceramics. Using various experimental techniques, we monitored the evolution of the structural, ferroelectric/dielectric, and electronic properties in our Ni-doped BaTiO3. We found that the reduction of Ti oxidation state by Ni doping plays a key role in the observed structural transition to h-BaTiO3. More details of our experimental results will be presented in conjunction with a discussion about the underlying mechanism of this polymorphic phase transition in BaTiO3.
8:00 PM - EL03.06.13
Three-Dimensional Atomic Scale Electron Density Reconstruction of Octahedral Tilt Epitaxy in Functional Perovskites
Yanfu Lu1,Yakun Yuan1,Venkatraman Gopalan1,Susan Sinnott1
The Pennsylvania State University1Show Abstract
Octahedral tilts are the most ubiquitous distortions in perovskite-related structures that can dramatically influence ferroelectric, magnetic, and electronic properties; yet the paradigm of tilt epitaxy in thin films is barely explored. Non-destructively characterizing such epitaxy in three-dimensions for low symmetry complex tilt systems composed of light anions is a formidable challenge. Here we demonstrate that the interfacial tilt epitaxy can transform ultrathin calcium titanate, a non-polar earth-abundant mineral, into high-temperature polar oxides that last above 900 K. The comprehensive picture of octahedral tilts and polar distortions is revealed by reconstructing the three-dimensional electron density maps across film-substrate interfaces with atomic resolution using coherent Bragg rod analysis. The results are in excellent agreement with density functional theory. The study could serve as a broader template for non-destructive, three-dimensional atomic resolution probing of complex low symmetry functional interfaces.
(1) Yuan Y, Lu Y, Stone G, et al. Nat. Commun. 2018, 9 (1).
(2) Haislmaier R, Lu Y, Lapano J, et al. APL Materials, 2019, 7 (5), DOI: 10.1063/1.5090798
8:00 PM - EL03.06.14
Advanced Techniques in Ultralow Voltage Piezoelectric Characterization of Ferroelectric Thin Films with Piezoresponse Force Microscopy
Aviram Bhalla-Levine1,Ryan Wu1,Sujit Das1,Roger Proksch2,Ramamoorthy Ramesh1
University of California, Berkeley1,Asylum Research2Show Abstract
There is currently significant interest in ultralow power microelectronics for memory and logic functions. Recent reports have identified multiferroic systems as possible candidates for such applications, with the ultimate goal of reducing the switching voltage to below one hundred millivolts (translating to approximately one attojoule per unit operation). Thus, measuring the ferroelectric and piezoelectric responses of ultrathin ferroelectric layers at such low voltage scales is essential. Piezoelectric measurements are, in principle, easier to execute and analyze since the primary response arises solely from the ferroelectric state (unlike polarization based measurements that are susceptible to leakage and nonlinear dielectric effects). To understand switching at voltages on the order of one hundred millivolts, we are carrying out a careful study of the piezoelectric switching of five, ten, fifteen, and twenty nanometer thick lead zirconate titanate films as a model system. We specifically focused on characterizing the piezoresponse of such nanoscale thin films using very low alternating current voltages (down to ten millivolt excitations). Our research indicates that statistically credible piezoelectric switching information can be obtained at these voltages. We will report the results of these scaling studies using piezoresponse force microscopy (PFM) as well as pulsed polarization measurements.
8:00 PM - EL03.06.15
New Lead-Free Materials on the Base of Sodium-Potassium Niobate and Sodium-Bismuth Titanate Perovskites
Karpov Institute of Physical Chemistry1Show Abstract
New Lead-Free Materials on the Base of Sodium-Potassium Niobate and Sodium-Bismuth Titanate Perovskites
E.D. Politova1, G.M. Kaleva1, A.V. Mosunov1, N.V. Sadovskaya1, S. Yu. Stefanovich1,2
D.A. Kiselev3, A.M. Kislyuk3, T.S. Ilina3,
1L.Ya.Karpov Institute of Physical Chemistry, Vorontsovo pole str. 10, Moscow 105064 Russia,
2Lomonosov Moscow State University, Leninskie gory 1, Moscow 119992 Russia,
3National University of Science and Technology “MISiS”, Leninskii pr. 4, Moscow 119991 Russia,
Lead-free materials are being intensively studied in order to replace widely used Pb-based ones. We study influence of cation substitutions and preparation conditions on structure parameters, microstructure, dielectric, relaxor ferroelectric, and piezoelectric properties of solid solutions in the systems based on (Na0..5Bi0.5)TiO3 (NBT) and (K0.5Na0.5)NbO3 (KNN) perovskites.
Ceramic samples in systems (Na0.5Bi0.5)TiO3 - BaTiO3 (NBT-BT) and (K0.5Na0.5)NbO3 – BaTiO3 (KNN-BT) with compositions close to Morphotropic Phase Boundaries (MPB) were prepared by the two-step solid-state reaction method at temperatures of 900 – 1500 K. To modify properties of the samples, in A- and B-sites of perovskite lattice Li+, La3+, Mn3+, Ni3+, Fe3+, Nb5+ , Sb5+ and W6+ cations were added. To improve density of ceramics overstoichiometric KCl and LiF additives were used.
The samples were characterized using the X-ray Diffraction, Scanning Electron Microscopy, Second Harmonic Generation (SHG), Dielectric Spectroscopy (DS), and Atomic Force Microscopy in Piezorespone Force mode (PFM) methods.
The unit cell volume changes were observed in modified KNN- and NBT-based ceramics depending on ionic radii of substituting cations. Ferroelectric phase transitions at ~ 400-500 and 600 – 700 K were confirmed using the DS and SHG methods. Phase transitions near ~ 400 K in NBT-based compositions revealed typical relaxor behavior due to the presence of polar nanoregions in a nonpolar matrix. At high temperatures > 700 K effects of dielectric relaxation were observed in ceramics studied caused by formation of oxygen vacancies in compositions with aliovalent substitutions. At the room temperature, non monotonous changes of the dielectric parameters and increase in the spontaneous polarization value was proved for modified ceramics. Using the PFM method ferroelectric polarization switching at nanoscale was observed, and in some KNN-based ceramics high values of effective d33 piezoelectric coefficient up to 300 pm/V were observed. The results obtained confirmed prospects of new lead-free materials development on the base of modified KNN- and NBT-based compositions.
Acknowledgment. The work was supported by the Russian Foundation for Basic Research (Project 18-03-00372).
8:00 PM - EL03.06.16
Giant Polarization in Super-Tetragonal Ferroelectric Thin Films through a New Concept of Interphase Strain
University of Science and Technology Beijing1Show Abstract
Generally, the chemical or physical properties strongly depend on the change of lattice. The control of lattice strain, therefore, much affects the chemical or physical properties of functional materials, which has been widely used in superconductivity, giant magnetoresistance, multiferroics, catalysis and etc. Ferroelectrics are an important functional material, which has been widely used in the field of ferroelectric memories, tunable microwave devices, large-capacity capacitors, piezoelectric sensor devices, etc. The intriguing properties of ferroelectric materials utilize the basic functional primitive parameter of polarization. This team has realized this method, interphase strain, by creating a single-lattice-parameter epitaxial composite film on SrTiO3 substrate from two tetragonal materials but with different lattice parameters, PbTiO3 ferroelectrics and PbO non-ferroelectrics. The results show that the method improves the lattice distortion of PbTiO3 to c/a = 1.238, compared to 1.065 in bulk. The remanent polarization is as high as 236.3 μC/cm2, which is near twice the highest value of the known ferroelectrics. This composite ferroelectric thin film is very stable, and the super-tetragonal ferroelectric phase is stable up to 725 °C, compared to the bulk transition temperature of 490 °C.
The proposed “interphase strain” is a new concept for strain engineering to regulate lattice strain of ferroelectrics, and successfully achieved giant polarization in the super tetragonal PbTiO3/PbO based ferroelectric thin films. The idea of "interphase strain" is as follows: if two kinds of materials with similar crystal structures, but different lattice parameters, are growing into a single-lattice-parameter epitaxial film, the material of the small lattice is inevitably subjected to the tensile stress from the large lattice material, thereby introducing a large lattice strain. The regulation of lattice strain can cause significant changes in the physical and chemical properties of the material. This new approach of interphase strain for strain engineering can be utilized to enhance the physical and chemical properties of other functional materials, such as superconductivity, giant magnetoresistance, multiferroic, and catalysis.
 Zhang L, Chen J, Fan L, et al. Giant polarization in super-tetragonal thin films through interphase strain[J]. Science, 2018, 361(6401): 494-497.
8:00 PM - EL03.06.17
In-Plane Ferroelectricity in Epitaxial Dion-Jacobson CsBiNb2O7
Jie Jiang1,2,Lifu Zhang1,Jian Shi1
Rensselaer Polytechnic Institute1,Kunming University of Science and Technology2Show Abstract
Conventional ferroelectric perovskite materials carry a debatable critical thickness below which the depolarization field is large enough to destabilize ferroelectricity. 2D ferroelectric materials are discovered to hold robust in-plane polarization down to a single unit cell, contending the continuous miniaturization of ferroelectric devices. However, due to the nonuniformity of the electrostatic field from quasi-2D metal electrodes, the in-plane intrinsic dipoles would experience a mismatched screening (screening frustration) making the in-plane polarization switching dynamics complex. Until now there is rare direct experimental proof of the in-plane polarization switching in a 2D crystal. In this talk, for the first time, we will present the in-plane polarization switching in a Dion-Jacobson quasi-2D layered oxide. The coupling between the in-plane ferroelectricity and other physical properties, e.g. the switchable photo diode effect and the photon-induced domain switching, in layered materials may enable versatile applications down to the atomic scale.
8:00 PM - EL03.06.18
Nontrivial Topological Polarization Field Self-Ordered in Nanoporous Ferroelectrics—A Phase-Field Modeling
Takahiro Shimada1,Le Van Lich1,2,Takayuki Kitamura1,Hiroyuki Hirakata1
Kyoto University1,Hanoi University of Science and Technology2Show Abstract
Topological objects or field textures, such as skyrmions, merons, and vortices, are intriguing features found in ordered systems with spontaneously broken symmetry. A plenty of topological field textures have been discovered, especially in magnetic and ordered soft matter systems, due to the existence of chiral interactions, and this has provided a fruitful platform for unearthing additional groundbreaking functionalities. However, despite one of the most important classes of ordered systems, ferroelectrics scarcely form topological polarization structures due to lack of such chiral interactions. Here, we show that a rich assortment of nontrivial topological polarization textures, including hedgehogs, antivortices, multidirectional vortices, and vortex arrays, can be spontaneously formed in three-dimensional nanoporous ferroelectric structures using the phase-field modelling based on the Ginzburg–Landau theory. We demonstrate that confining ferroelectrics to trivial geometries that are incompatible with the orientation symmetry may impose extrinsic frustration to the polarization field through the enhancement of depolarization fields at free porous surfaces. This frustration yields symmetry breaking, resulting in the formation of nontrivial topological polarization field textures. We also characterize the topological feature of polarization structures according to the topological theory of defects and homotopy theory. The results indicate that the nanoporous structures possess topological objects composed of two or more elementary topological polarization structures. This study therefore offers an intriguing playground for exploring novel physical phenomena in ferroelectric systems as well as a novel nanoelectronics characterization platform for future topology-based nanotechnologies.
8:00 PM - EL03.06.19
Frustrated Dipole Order Induces Noncollinear Proper Ferrielectricity in Two-Dimensions
Ling-Fang Lin1,2,3,Yang Zhang1,2,3,Shuai Dong1
Southeast University1,The University of Tennessee, Knoxville2,Oak Ridge National Laboratory3Show Abstract
Within Landau theory, magnetism and polarity are homotopic, displaying a one-to-one correspondence between most physical characteristics. However, despite widely reported noncollinear magnetism, spontaneous noncollinear electric dipole order as ground state is rare. Here a dioxydihalides MO2X2 family (layered structure, where M= Mo and W; X= Cl and Br) is predicted to display noncollinear ferrielectricity, induced by competing ferroelectric and antiferroelectric soft modes. This intrinsic noncollinearity of dipoles generates unique physical properties, such as Z2×Z2 topological domains, atomic-scale dipole vortices, and negative piezoelectricity.
8:00 PM - EL03.06.20
Defect Complex and Hopping Mechanism in (Li, Al) Co-Doped ZnO Ceramics
Dong Huang1,Francis Chi Chung Ling1
The University of Hong Kong1Show Abstract
Systematic studies on sintering temperature and Li:Al stoichiometry of Li and Al co-doped ZnO ceramic shows that the Zn0.99(Li0.1, Al0.2)0.033O sample exhibits a colossal dielectric constant (CDC) phenomenon with low dielectric loss ( and =0.159 at the frequency of 1 kHz) at the room-temperature. The CDC and low dielectric loss have good frequency stability. SEM and CL measurements show the grain boundary of the as-grown LAZ sample is accumulated with high density of VO, and the spatial non-uniformity of VO concentration is removed after the O2 annealing. With the impedance analysis, it is shown that the RGD (resistance of grain boundaries) is only ~16 times larger than RG (resistance of grain), and the CPEGD is even smaller than CPEG, implying that internal barrier layer capacitance (IBLC) effect is not likely the dominant source for the observed CDC of the LAZ samples. Dielectric spectrum analysis shows that the CDC is associated with two relaxation processes P1 and P2. Annealing the sample at 900 oC in oxygen leads to the drop of to 2250 but maintaining a low dielectric loss of ~0.10, while P1 vanishes and P2 persists. Comparing the synchrotron based hyperfine Al 2p X-ray photoelectron (XPS) spectra of the purely Al-doped ZnO sample and the Li+Al co-doped ZnO sample shows that the electronic environment around the AlZn in these two samples are different, indicating that defect complex consisting of AlZn and LiZn is probably presence in the Li+Al co-doped sample. Furthermore, after the Raman comparisons among the co-doped, singly Li- or Al- doped ZnO, it is shown the defect complex has altered the Zn-O bond’s local environment, which lead to the shift of A1 stretching mode. This defect complex is possibly the electron pinning defect dipole responsible for the CDC associated with the P2 relaxation process. With the correlated barrier hopping model fitting, it is found that two energy level EC-0.34 eV and EC-0.87 eV are existed in as grown and O2 annealed LAZ sample, causing the P1 and P2 relaxation, respectively. With two potential well model, we theoretically calculate the dielectric constant and loss against frequency for P1 and P2 relaxation, which are around ~7173 and ~2817.
8:00 PM - EL03.06.22
Structure-Property Correlation in the Multiferroic (Bi1-xBax)(Fe1-xTix)O3 System
Arun Kumar1,Dhananjai Pandey1
Indian Institute of Technology (BHU)1Show Abstract
Magnetoelectric multiferroics offer the possibility of controlling the electric (magnetic) polarization by applying a magnetic (electric) field and have attracted significant interest in view of the interesting physics of coupling between magnetic and ferroelectric order parameters and potential technological applications in several multifunctional devices. BiFeO3 is unique amongst various magnetoelectric multiferroics, as its ferroelectric and magnetic transition temperatures (TC ~1103 K, TN ~643 K) are well above the room temperature. In recent years, the (Bi1-xBax)(Fe1-xTix)O3 (BF-xBT) system have received considerable attention due to large ferroelectric polarization, large remnant magnetization, linear magnetoelectric coupling and highest depolarization temperature for piezoelectric applications and considered to be alternative to toxic lead (Pb) containing piezoelectric ceramics like Pb(ZrxTi1-x)O3 and (1-x)Pb(Mg1/3Nb2/3)O3-xPbTiO3. In the present investigation, we have carried out a comprehensive study on 0.3 wt% Mn-doped BF-xBT samples in the composition range 0≤ x ≤1.0. Our synchrotron x-ray diffraction results reveal two structural phase boundaries, one from rhombohedral (R3c space group) to cubic (Pm-3m space group) at xc1~0.33 and other from cubic (Pm-3m space group) to tetragonal (P4mm space group) at xc2~0.80. The composition dependence of the polarization and dielectric constant at room temperature exhibits a peak around x=0.33. This confirms the existence of morphotropic phase boundary at this composition due to a rhombohedral (R3c) to cubic (Pm-3m) phase transition across the morphotropic phase boundary. We also present a magnetic phase diagram of BF-xBT.
8:00 PM - EL03.06.23
Phase-Field Simulation and High-Throughput Calculation of Resistive Switching Behavior in Random Access Memory
Ye Cao1,Kena Zhang1,Jianjun Wang2
The University of Texas at Arlington1,The Pennsylvania State University2Show Abstract
Metal-oxide based Resistive Random-Access-Memory (RRAM) which exhibits multiple resistive/memory states by the formation/dissolution of a conductive filament (CF), has potential to be the next generation memory technology. The performance of RRAM relies on the fast switching speed, large current on/off ratio, and minimized device variability, which are critically dependent on the ion (such as oxygen vacancies) migration driven by the concentration gradient, electrical bias, hear generation and dissipation. In this work we report that the mechanical stress induced by the growth and retraction of the conductive filament is equally important to the resistive switching dynamics. The stress inhibits the ion diffusion and segregation along the electric field direction and reduces the current on/off ratio and the switching time. To further understand the role of this mechanical stress in the resistive switching process, we developed a comprehensive phase-field model taking into account the electrical, thermal, and mechanical energy, and studied their relative effects on the RRAM resistive switching dynamics. We choose hafnium oxide as an example, and compare the simulation results with existing experimental results to validate the model. Based on this, high-throughput phase-field simulations for different oxides of different properties are performed to help selecting the potential candidates as the oxide switching layer materials with optimized switching speed, current on/off ratio and device uniformity. Our work thus provides fundamental insights into the resistive switching mechanism, and establishes a theoretical framework of materials selection and design for metal-oxide based RRAMs.
8:00 PM - EL03.06.24
Symmetry Mismatch at Heterointerfaces and Photovoltaic Effect in BiFeO3/LaFeO3 Ferroïc Superlattices
Mimoun El Marssi1,Jamal Belhadi1,Said Yousfi1,Benjamin Carcan1,Houssny Bouyanfif1
University of Picardy1Show Abstract
Bismuth ferrite (BiFeO3 or BFO) is the most studied multiferroic due to its robust ferroelectric state coexisting at room temperature with an antiferromagnetic order. Such coexistence and the possible cross coupling between both ferroic orders pave the way to so-called MagnetoElectric RAM combining advantages of the ferroelectric and the antiferromagnetic state. Similarly to the relaxor-ferroelectric systems a morphotropic phase boundary has been observed in La doped BFO (Bi,La)FeO3 solid solution with peculiar nanoscale mixture. Emergence of such MPB is believed to arise from the competition between antiferrodistortive and ferroelectric instabilities. Our approach to investigate the structural interaction between BFO and LFO is based on superlattices that are ideal platforms for exploring antagonistic interactions at the origin of many exotic systems. For instance Cuprates combined with Manganites in superlattices were investigated to better understand the competition between magnetic and superconducting orders. Similarly to this strategy we grew series of SLs made of BiFeO3 and LaFeO3. Structural characterizations and Raman spectroscopy indicate an anti-polar structure in the BFO layers that is strongly dependent on the BFO thickness and temperature [1,2]. This antiferroelectric like structure very similar to the PbZrO3 system cannot be explained by the nature of the induced strain but by the symmetry mismatch at the interfaces of the SLs. Compatibility of the octahedral tilt system seems to be the main driving force for this induced anti-polar state. Thickness-temperature phase diagram is constructed.
We have highlighted a switchable PV effect in these artificial structures at room temperature. By changing the thickness of the BFO layer we have evidenced a change of PV characteristics from a positive Voc and a negative Jsc to an inverse effect. These results, compared to our results obtained on BFO single films , indicate different origin of the mechanisms of photo-carries separation in PV devices. Our results are promising and indicate the possibility to employing the vertical geometry of measurements for tuning the PV effect in multiferroic SLs.
 B. Carcan et al., Adv. Mater. Interfaces, 4, 1601036 (2017)
 B. Carcan et al., Journal of Applied Physics 124, 044105 (2018)
 J. Belhadi et al. Journal of Physics: Condensed Matter, 31, 275701 (2019)
8:00 PM - EL03.06.25
Effect of Quadravalent Heavy Transition Metal Cations on Microwave Properties of Co2Z Ferrites
Piotr Kulik1,Gavin Winter1,Katherine Murphy1,Jason Adams1,Ogheneyunume Fitchorova1,Vincent Harris1
Northeastern University1Show Abstract
The demand for miniaturized and high performing broadband communication systems in the GHz frequency range is steadily growing due to severely crowded and rapidly changing modern commercial and military spectral environments. Hexaferrite composites have proven to be one of the few key enablers in providing miniaturized form factors due to their high permeability and permittivity as well as their capability to reach high resonance frequencies up to 100 GHz. In this work, a series of Z-type barium hexaferrites were prepared in which dopants of heavy transition metals, i.e., Mo4+ and Hf4+, were employed to modify structure and microwave properties. Through systematic measurements it was revealed that each dopant affected the hexaferrites’ properties differently by both shifting the resonant frequency and altering magnetic properties without strongly varying the hexaferrite crystallographic structure. Additionally, ε' = μ' was realized without any additives such as Bi2O2, which had been previously been used for tuning permeability and permittivity. Polycrystalline Co2Z ferrites, having a nominal composition of Ba3Co2+XHfXFe24-2XO41 and Ba3Co2+XMoXFe24-2XO41, where x=0 to 0.05, were prepared by a solid-state process. BaCo3, HfO2, MoO2, Co3O4, and Fe2O3 of high purity were mixed and calcined in oxygen for 5-8 hours at 800-1050 °C, which then were ball milled for 18-24 hours to reduce the grain size to under 1 µm. After ball-milling, ISOBAM was added as a binder and mixed for several minutes. Samples were then pressed to form toroids with an inner diameter of 3 mm and an outer diameter of 7 mm. The toroids were pressed by a cold isostatic press in order to maximize compaction before sintering in oxygen for 4-6 hours at 1000-1250 °C. Finally, samples were measured using the Agilent E864A PNA and a 7 mm precision airline, showing permeability and frequency changes. Results show that a nine-time reduction in size can be achieved while maintaining an impedance of 360 Ω close to that of free space over a broadband.
8:00 PM - EL03.06.26
Insights into Magneto-Electric Coupling Using X-Ray Photoemission Electron Spectro-Microscopy
Lawrence Berkeley National Laboratory1Show Abstract
Ferromagnetic-ferroelectric (FM-FE) heterostructures have been studied as a route to obtain strong room-temperature magneto-electric interactions not commonly found in single-phase materials.1 In such composites it is critical to understand the role of charge- and strain- mediated interactions at interfaces of the constituent phases, and spatially resolved probes such as x-ray photoemission electron microscopy (XPEEM) at the Advanced Light Source PEEM-3 beamline can observe such interface interactions at the scale of a single FE or FM domain. Polarization-dependent soft x-ray spectro-microscopy as a function of temperature and applied electric and magnetic fields can offer unique insights into coupling at heterointerfaces with sub-100 nm resolution by exploiting the x-ray linear dichroism (XLD) and magnetic circular dichroism (XMCD) effects. I will present a detailed analysis of the magneto-electric coupling in model multiferroic systems (e.g. FM layers grown on FE single crystals, or single phase multiferroic epitaxial thin films) using XLD- and XMCD-PEEM imaging. While the 3D vector orientation of ferromagnetic domains can be mapped with XMCD imaging at different azimuthal orientations, anisotropic strain interactions between FE and FM phases can be mapped by XLD imaging in an analogous fashion.2,3 The anisotropic nature of the strain imprinted by the FE induces a local variation of the magnetic anisotropy of the FM phase due to large magnetoelastic anisotropy, and by varying applied electric fields or changes in temperature we can observe both the FM domain structure and imprinted strain state evolve due to such pertubations.2 Furthermore, we can compare spatially averaged electric-field dependent magnetometry to spatially resolved XMCD images in applied magnetic fields, and directly correlate a giant anisotropy rotation and change of anisotropy symmetry to the local tuning of magnetic anisotropy at the scale of single FE and FM domains.3 Similarly, PEEM-based mapping of multiple ferroic orders can offer insight into optical switching mechanicsms of single-phase multiferroic materials.4 Thus, XLD- and XMCD-PEEM imaging offer a facile method to visualize magnetoelectric coupling at the sub-micron scale by probing FE, FM, or antiferromagnetic domain evolution as a function of stimuli such as in situ applied electric or magnetic fields.
1. W. Eerenstein and N. Mathur, Nature 442, 759 (2006).
2. R. V. Chopdekar et al, Phys. Rev. B 86, 014408 (2012).
3. R. V. Chopdekar et al, Sci. Rep. 6 27501 (2016).
4. Liou et al, Nat. Mater. 18 580 (2019).
8:00 PM - EL03.06.27
MoS2 Negative Capacitance Field-Effect Transistor Based on PLD Grown Hf0.5Zr0.5O2
Hae Won Cho1,Seongin Hong1,Junwoo Park1,Sunkook Kim1,Jeonghyeon Oh
Sungkyunkwan University1Show Abstract
Recently, the power consumption density has increased compared to the transistor which has increased exponentially per unit chip, making it difficult to store and process a large amount of data. Therefore, the development of low-power semiconductor technology is inevitable. In order to solve this issue on power consumption, research on a negative capacitance field-effect transistor (NCFET) is being actively conducted. In case of metal oxide semiconductor field-effect transistor (MOSFET), which is a conventional CMOS device, the subthreshold slope (S.S) value cannot fall below 60 mV/decade. NCFET, the next generation low-power device to replace MOSFET that encounters this limitation, can dramatically reduce power consumption density. Ferroelectric is negative capacitor in the gate structure of the NCFET, allowing channel surface potential to be amplified more than the gate voltage, enabling drive at less than 60 mV/dec S.S at room temperature. In this study, the ferroelectric Hf0.5Zr0.5O2 (HZO) material in the gate structure was grown through pulsed laser deposition (PLD) process, and MoS2 was used as a channel material to develop low power, high mobility 2D-NCFET. Conventionally, the ferroelectric HZO grown by atomic layer deposition (ALD), has been widely studied in electronic device development. In addition, research has been carried out focusing on HZO epitaxial growth at various substrates by PLD process. For the first time, we have introduced a new process to operate MoS2 NCFET based on HZO, grown on Si substrate by PLD. The process conditions such as oxygen partial pressure were controlled during the experiment, and the Al2O3 (k~9) as bottom dielectric layer scaling resulted in a five-fold improvement in the subthreshold slope (S.S), operating the device at low power, from approximately 500 mV/dec to 100 mV/dec. To develop low power devices obtaining less than 60 mV/dec, the PLD process will further be optimized for the enhancement of ferroelectricity to obtain larger NC effect.
8:00 PM - EL03.06.28
Anomalous Remnant Magnetization in Gadolinia Nanospindles at Room Temperature?
Parvez Akhtar1,Sandeep Kumar1,Madhusudan Singh1
Indian Institute of Technology Delhi1Show Abstract
Gadolinium oxide (Gd2O3) is expected to exhibit strong interactions with external magnetic fields due to the high magnetic moment of Gd (7.94 µB). Applications range from a positive contrast agent in magnetic resonance imaging (MRI) to use as a cooling agent in magnetocaloric effect (MCE) based refrigerators. In this work, we report on the preparation of Gd2O3 nanospindles by a hydrothermal method, followed by measurement of its mass magnetization. Powdered Gd2O3 source (CAS: 12064-62-9, 99.9% trace metals basis, Sigma-Aldrich) was subjected to aqueous colloidal hydrothermal synthesis and subsequently annealed at 500oC to produce cubic phase (JCPDS: 882165) Gd2O3, inferred from powder X-ray diffraction (PXRD, Advance Bruker D8, Ni-filtered Cu Kα radiation (λ = 1.5418 Å)). The morphology of nano-spindles (length ~100 ± 10 nm) was studied by field-emission scanning electron microscopy (FESEM-FEI QUANTA 3D FEG). Raman spectra confirmed the cubic phase of Gd2O3 with a highly intense and characteristic peak at 361 cm-1. A small quantity of the product (1.23 mg) was wrapped in Teflon tape and exposed to magnetic fields in the range [-2,2] kOe in an Alternating Gradient Magnetometer (Micromag 2900 PMC) at room temperature. Measurements of magnetic moment (emu), converted into mass magnetization (emu/g), exhibit a quasi-saturated hysteresis behavior at limits of magnetic field excitation. The saturation magnetization (Ms), retentivity (Mr) and coercivity (Hc) are found to be 540.809 ± 4.381 m emu/g, 23.348 ± 0.186 m emu/g, and 21.218 ± 1.024 Oe, respectively over multiple measurements. The absence of saturation at the applied field in the magnetic hysteresis (M-H) curve suggests a mix of paramagnetic (PM) and ferromagnetic (FM) phases at room temperature. We are performing further materials analysis and investigating this magnetization result at different temperatures to validate it, and to understand the precise mechanism, in light of known defect-induced magnetization in various materials, albeit at lower temperatures. Potential applications include possible low-cost solution-processable magnetic devices and sensors.
8:00 PM - EL03.06.29
Enhanced Gilbert Damping in Sputter Deposited Topological Insulator/Ferromagnet Heterostructures
Nirjhar Bhattacharjee1,Ivan Lisenkov2,Alexandria Will-Cole1,Jiawei Wang1,Nian Sun1,2
Northeastern University1,Winchester Technologies, LLC2Show Abstract
Topological insulators (TI) have been known to possess topologically protected surface conducting states  and Rashba 2D electron gas (2DEG) due to band bending at interfaces . A TI placed in contact with a ferromagnetic (FM) metal generates spin-orbit torques (SOT) on the magnetization in FM [2,3]. A signature of SOT in TI/FM bilayers is an increase in Gilbert damping in FM. SOT in TI/FM (ferromagnet) films have been reported previously with TI films epitaxially grown with molecular beam epitaxy [2, 3]. Here we report enhanced Gilbert damping in sputter deposited TI/FM, BixTe(1-x)/CoFeB (BT/CFB) films (x = ~0.4). Samples of 20nm BT film were grown on a Si/SiO2 substrate at 250C and at 30C followed by 20nm CFB deposition at 30C (room temperature) using RF and DC magnetron sputtering respectively. X-ray diffraction (XRD) measurements reveal a crystalline 250C BT film compared to an amorphous 30C BT film. Room temperature broadband ferromagnetic resonance (FMR) measurements were conducted for 250C and 30C heterostructures and a control sample where the TI was substituted with 3nm Al. A full width at half maximum (FWHM) resonance linewidth was extracted as a function of frequency to calculate Gilbert damping. The control and 30C samples show almost identical linewidth, but the 250C sample linewidth is much broader. The Gilbert damping coefficient, α, for 250C sample is α = 0.3, compared to α = 0.03 for 30°C and α = 0.02 for control. The calculated spin-mixing conductance for 250C sample is g = 4e21 m-2 which is in an order of magnitude higher than reported value for CFB/Pt films . Moreover, the presence the crystalline TI film adjacent to FM induces static effects on the magnetization. M-H loop measurements reveal emergence of out of plane magnetic anisotropy (OPMA) for the 250C sample at lower thicknesses (<5nm) of CFB films. This change in the magnetic anisotropy and spin pumping in the BT/CFB heterostructure is attributed to presence Rashba 2DEG because of strong spin-orbit coupling [5-8] at the interface, which is enhanced for the crystalline phase of BT. Further, spin-torque FMR studies on our samples is being carried out to characterize the effects on magnetization dynamics due to sputtered TI/FM interfaces.
1.Y. L. Chen, J. G Anaytis and J. -H. Chu et al., Science Vol. 325, p. 5937 (2009).
2. A. R. Mellnik, J. S. Lee and A. Richardella et al., Nature Vol. 511, p. 449 (2014).
3. J. Han, A. Richardella and S. A. Siddiqui et al., Phys. Rev. Lett. Vol. 119, p. 077702 (2017).
4. M Belmeguenai, M. S. Gabor and F. Xigheim et al., J. Phys. D: Appl. Phys. Vol. 51 p. 045002 (2018).
5. A. Manchon, H. C. Koo and J. Nitta et al., Nature Materials Vol. 14, p. 871 (2015).
6. F. Khatmis, V. Lauter and F.S Nogueira et al., Nature, Vol 533, 513 (2016).
7. J. Kim, K, W. Kim and R. Wu et al., Phys. Rev. Lett. 119, 027201 (2017).
8. M. S. Bahramy, P.D.C. King and A. de la Torre et al., Nature Comm Vol 3, 1159 (2012).
8:00 PM - EL03.06.30
Substrate-Modulated Ferromagnetism of Two-Dimensional Fe3GeTe2
Luyao Song1,Luman Zhang1,Xinyu Huang1,Lei Ye1,Junbo Han1
Huazhong University of Science and Technology1Show Abstract
Ferromagnetism in two-dimensional (2D) Van der Waals materials promises to revolutionize and develop spintronic devices and has received increased attention due to the electrical stability and sensitive tunability of an external field. To achieve high performance in spintronic devices, the effect of device substrates on the ferromagnetism of 2D materials also plays a critical role in practical device design and fabrication but has not yet been examined. Here, we systematically demonstrated the substrate-modulated ferromagnetism of 2D Fe3GeTe2 based on different substrates. The out-of-plane ferromagnetism of Fe3GeTe2 thin films prepared on Al, SiO2 and Au substrates was probed using Magneto-optical Kerr effect techniques. Based on the experimental data, Fe3GeTe2 thin films with the same thickness were modulated to show different TC on different substrates, with the highest TC on Au substrate, especially in a thin layer. The underlying reason was explained by the first-principle calculation and mean field approximation, revealing that the charge redistribution and lattice distortion play an important role on magnetic properties changes. Our work provides a practical way to modulate the magnetic properties of ferromagnetic materials permanently without applying any additional treatment processes, and a feasible theoretical method to study the fundamental physical properties of ferromagnetic materials.
Nian Sun, Northeastern University
Jane Chang, University of California, Los Angeles
Shashank Priya, The Pennsylvania State University
Eckhard Quandt, University of Kiel
EL03.07: Multiferroics III
Wednesday AM, December 04, 2019
Hynes, Level 1, Room 101
8:30 AM - EL03.07.01
Electrically Reversible Spin Texture in Ferroelectric Oxides
University of Nebraska-Lincoln1Show Abstract
Spin-orbit coupling is known to be responsible for non-trivial spin configurations and a number of emergent physical phenomena. Ferroelectric materials are especially interesting in this regard due to broken space inversion symmetry, which enforces the emergence of the bulk Rashba and Dresselhaus spin-orbit coupling, and reversible spontaneous polarization, which allows for a non-volatile electrical control of the spin degrees of freedom. This talk addresses two classes of ferroelectric oxide materials exhibiting dissimilar spin textures due to different space-group symmetries. First, we consider a technologically relevant oxide material, HfO2, which is known to be ferroelectric in a non-centrosymmetric orthorhombic phase. We show that HfO2 exhibits Dresselhaus-type spin texture driven by spin-orbit coupling,1 and argue that this material can be used as a tunnel barrier to produce tunnelling anomalous and spin Hall effects that are reversible by ferroelectric polarization.2 Another example involves a class of materials capable to maintain a persistent spin texture. This property has been predicted to support an extraordinarily long spin lifetime of carriers promising for spintronics applications. We show that the persistent spin texture can be enforced by non-symmorphic space-group symmetry of the crystal, which makes it a robust intrinsic property of the bulk material.3 Using symmetry analyses and theoretical modelling based on density-functional theory, we demonstrate this property for a handful of oxide materials, which can be synthesized in laboratory. Among them BiInO3, a wide band gap ferroelectric semiconductor, is the most promising candidate which sustains persistent spin texture around the conduction band minimum. The reversible spontaneous polarization of BiInO3, allows for an electrical control of the spin polarization, which can be selectively induced by circular polarized optical pumping.
1. L. L. Tao, T. R. Paudel, A. A. Kovalev, and E. Y. Tsymbal, Reversible spin texture in ferroelectric HfO2, Physical Review B 95, 245141 (2017).
2. M. Y. Zhuravlev, A. Alexandrov, L. L. Tao, and E. Y. Tsymbal, Tunneling anomalous Hall effect in a ferroelectric tunnel junction, Applied Physics Letters 113, 172405 (2018).
3. L. L. Tao and E. Y. Tsymbal, Persistent spin texture enforced by symmetry, Nature Communications 9, 2763 (2018).
9:00 AM - EL03.07.02
Tunable Magnetotransport Properties of Epitaxial Nanocomposite Films
Quanxi Jia4,Aiping Chen1,Haiyan Wang2,Judith MacManus-Driscoll3
Los Alamos National Laboratory1,Purdue University2,University of Cambridge3,University at Buffalo, The State University of New York4Show Abstract
Over the past two decades, new discoveries and major advances have been made to enhance controlled synthesis of epitaxial ferromagnetic oxide films and to gain fundamental understanding of their physical properties. Tunable magetotransport properties, in particular, have been achieved through interfacing ferromagnetic materials with binary oxides at the nanoscale by forming nanocomposite films, where both the ferromagnetic and binary oxides are of nanoscale dimensions. In this talk, we will overview our strategies in synthesis and characterization of epitaxial magnetic nanocomposite films. Using controlled synthesis, advanced probing, and theoretical modeling, we are able to understand the effect of interface strain on the magnetotransport properties of ferromagnetic materials such as La0.7Sr0.3MnO3 films.
9:30 AM - EL03.07.03
Magnetoelectric Coupling by Giant Piezoelectric Tensor Design
University of Wisconsin--Madison1Show Abstract
Strain-coupled magnetoelectric (ME) phenomena in piezoelectric / ferromagnetic thin-film bilayers are a promising paradigm for sensors and information storage devices, where strain manipulates the magnetization of the ferromagnetic film. In-plane magnetization rotation with an electric field across the film thickness has been challenging due to the virtual elimination of in-plane piezoelectric strain by substrate clamping, and in two-terminal devices, the requirement of anisotropic in-plane strain. We have overcome both of these limitations with lithographically patterned devices with a piezoelectric membrane on a soft substrate platform, in which in-plane strain is freely generated, and a patterned edge constraint that transforms the nominally isotropic piezoelectric strain into the required uniaxial strain. We fabricated 500 nm thick, (001) oriented [Pb(Mg1/3Nb2/3)O3]0.7-[PbTiO3]0.3 (PMN-PT) unclamped piezoelectric membranes with ferromagnetic Ni overlayers. Guided by analytical and numerical continuum elastic calculations, we designed and fabricated two-terminal devices exhibiting Ni magnetization rotation in response to an electric field across the PMN-PT. Similar membrane heterostructures could be used to apply designed strain patterns to many other materials systems to control properties such as superconductivity, band topology, conductivity, and optical response.
This work has been done in collaboration with J. Irwin, S. Lindemann, W. Maeng, J. J. Wang, V. Vaithyanathan, J.M. Hu, L.Q. Chen, D.G. Schlom, C.B. Eom, M.S. Rzchowski.
This work was supported by the Army Research Office through grant W911NF-17-1-0462.
10:30 AM - EL03.07.04
Towards Low-Voltage Multiferroic/Magnetoelectric Operation
University of California, Berkeley1,Lawrence Berkeley National Laboratory2Show Abstract
Applications in advanced, beyond Moore’s law computing are driving researchers and industry alike to explore a broader set of materials than ever before. While industry has maintained, in some form, their ability to continually meet the demands of Moore’s law by increasing the number of transistors on chip, largely in part from efforts in scaling and size reduction of the transistors themselves and the associated circuit area, the same cannot be said for energy scaling. In the last fifteen years, scaling has deviated from Dennard’s trend which states that the power density of circuits stays roughly the same as transistors get smaller, assuming, concurrent voltage reductions are made. Herein lies the challenge – while we have reduced transistor and circuit size, voltages of operation have not been scaled at the same rate. As a result, power and energy dissipation now stands as one of the most pressing challenges for advanced nanoelectronics. This has motivated renewed attention to a wide variety of routes to reduce the voltage of operation of next-generation logic. Such approaches have thrust materials – including multiferroics and magnetoelectrics – back into the mix as candidates for beyond CMOS computing.
Despite considerable research on multiferroic and magnetoelectric materials in the last decade and advances in our ability to synthesize, control, characterize, and fabricate these materials, the requirements of beyond Moore’s law computing are already pushing these materials to their limits. In this talk, we will explore recent efforts to reduce the operating voltages of multiferroic and magnetoelectric devices including exploring both new and old materials in ever decreasing sizes. In particular, we will explore efforts to push the size limits of these materials whereby reducing the thickness of films provides a direct pathway to reduced operation voltages. Special attention will be given to challenges in achieving ultra-thin-film operation in multiferroics such as BiFeO3 and Bi1-xLaxFeO3 as well as in magnetoelectric composite structures based on piezoelectric/ferroelectric materials such as BaTiO3 and (1-x)PbMg1/3Nb2/3O3-(x)PbTiO3 (PMN-PT). For example, while considerable work has been done in PMN-PT as bulk ceramics, single crystals, and thick films, essentially no work on ultra-thin films has been considered. We will explore the evolution of relaxor order and actuation potential as we reduce relaxor film thicknesses to the range of 5-100 nm. Studies suggest surprising enhancement of relaxor character with reducing thickness and the presence of a complex, thickness evolution to structure and properties. We will explore other approaches including orientation dependence and chemical routes to reduce polarization or manipulate structure in such as fashion that it reduces the costs of switching polarization. For example, in PbZr0.2Ti0.8O3 thin films, it has been shown that merely changing film orientation from (001)- to (111)-oriented structures can dramatically change coercive field scaling (thus avoiding classical Janovec-Kay-Dunn scaling trends) as a result of changes in materials symmetry which produce low-energy switching pathways. Finally, we will explore the effects of these approaches on the realization of low-voltage magnetoelectric coupling in heterostructures such as BiFeO3-based spin valves and composite ferromagnet/piezoelectric stacks. To end, we will discus where these ideas could lead us next and what metrics can be met using these materials and methods.
11:00 AM - EL03.07.05
Voltage Controlled Néel Vector Switching in High-TN Magnetoelectric Thin Films
Christian Binek1,Ather Mahmood1,Will Echtenkamp1,Junlei Wang1,Takashi Komesu1,Peter Dowben1
University of Nebraska-Lincoln1Show Abstract
Voltage-controlled magnetization switching at interfaces or boundaries enables dissipationless control of remnant magnetic states. It paves the way towards ultra-low power and non-volatile spintronics. We exploit substitutional Boron doping of the magnetoelectric antiferromagnet Cr2O3 to fabricate voltage switchable all antiferromagnetic memory devices which operate between room temperature and 400K, i.e., significantly above the antiferromagnetic ordering temperature TN = 307 K of pure Cr2O3. TN-enhanced and anisotropy reduced magnetoelectric films are grown via pulsed laser deposition in the presence of borane background gases. Boundary magnetization associated with two degenerate orientations of the Néel vector serves as state variable which can be isothermally written and read out. Writing is achieved through voltage-controlled switching of the Néel vector. Read out takes place by sensing an anomalous Hall-like signal originating from an electric current driven through a lithographically patterned Pt Hall bar deposited on top of the B-doped Cr2O3 film. In device architectures based on voltage-controlled exchange bias where remnant magnetization of a ferromagnetic film serves as state variable, B-doping does not translate into improved performance. Although B-doping can increase the blocking temperature, exchange coupling is not accompanied by effective pinning and thus voltage-control of the ferromagnet. The detrimental effect of B-doping on perpendicular exchange bias is attributed to reduced magnetic anisotropy and canting of the interface magnetization relative to the surface normal. It takes place despite perseverance of antiferromagnetic order and magnetoelectric functionality above 307 K as evidenced by magnetometry and photoemission spectroscopy. In contrast to pure chromia, where order parameter switching is controlled by the competition between magnetoelectric and anisotropy energy, the switching mechanism in B-doped chromia seems to be additionally affected by a sizable electric field dependence of the magnetic anisotropy. Our results demonstrate that TN-enhancement and anisotropy reduction through B-doping of Cr2O3 is successfully utilized in voltage-controlled spintronic devices with reduced complexity. Our Hall bar structures based on B-doped chromia show voltage-controlled switching up to 100 K above room temperature paving the way to CMOS compatible ultra-low power magnetoelectric MRAM and logic devices.
We acknowledge support by SRC and NSF through ECCS 1740136, MRSEC DMR-1420645, and NNF under Award NNCI: 1542182 and support by ARO through MURI W(11NF-16-1-0472.
11:30 AM - EL03.07.06
SHG-Active Boundaries between Nonpolar Magnetic Domains in MnWO4
Shingo Toyoda1,Manfred Fiebig1,2,Takahisa Arima1,3,Yoshinori Tokura1,3,Naoki Ogawa1,4
RIKEN CEMS1,ETH Zürich2,The University of Tokyo3,JST PRESTO4Show Abstract
Domain walls often show a novel functionality very different from that of bulk states. Despite their importance, the domain wall physics are not well understood compared to the bulk cases because of the lack of experimental techniques to investigate the confined walls. In the present study, we conducted a SHG imaging measurement which allows us to probe the domain walls in MnWO4. We found multiferroic domain walls in a non-multiferroic environment.
MnWO4 crystalizes in a centrosymmetric space-group P2/c, and shows successive magnetic phase transitions below the Néel temperature TN = 13.5 K. In the AF2 phase, the magnetic order breaks the space-inversion symmetry and ferroelectric polarization appears along the b-axis , while the other phases have non-polar magnetic structures. Correspondingly, SHG is allowed only in the AF2 phase, while it is forbidden in the AF1 and AF3 phases. However, it was found that non-zero SHG signal exists even in the SHG-forbidden AF1 phase . We revealed that the SHG signal in the AF1 phase comes from wall-like structures. Polarization anisotropy and spectroscopy measurements of the SHG signal suggest that the wall in the AF1 phase should have a magnetic structure similar to that of the multiferroic AF2 phase. The results indicate the existence of domain walls breaking space-inversion symmetry, although the bulk phase is centrosymmetric. We propose the emergence of multiferroic domain walls in a non-multiferroic environment.
 K. Taniguchi et al., Phys. Rev. Lett. 97, 097203 (2006).
 D. Meier et al., Phys. Rev. B 80, 224420 (2009).
11:45 AM - EL03.07.07
A Dynamical Magnetic Field Accompanying the Motion of Ferroelectric Domain Walls
Dominik Juraschek1,2,Quintin Meier2,Morgan Trassin2,Susan Trolier-McKinstry3,Christian Degen2,Nicola Spaldin2
Harvard University1,ETH Zürich2,The Pennsylvania State University3Show Abstract
The domain walls that separate different orientations of electric polarization in ferroelectric materials have long been of interest because their motion governs the process of ferroelectric switching in an electric field . Recently, a range of unexpected behaviors have been discovered at domain walls that do not occur in the bulk of the domains, such as ferrielectricity, magnetoelectricity, and electrical conductivity or even superconductivity, suggesting additional interest in domain walls as functional entities in their own right .
At the same time, the magnetization caused by the usual motion of electric charges has been revisited over the last years in the context of time-varying ferroelectric polarizations. This newly described dynamical multiferroicity, associates a magnetization M of the form M ~ P × ∂t P with a ferroelectric polarization P. A range of existing coupled electric-magnetic phenomena fall within the dynamical multiferroicity framework, and new behaviors, including a phonon Zeeman effect, exotic quantum criticality and phonon orbital magnetism have been proposed [3-5].
Here we establish the link between these two concepts -- dynamical multiferroicity and ferroelectric domain wall functionality -- by showing theoretically that the motion of ferroelectric domain walls can be accompanied by a dynamical magnetic field. We extend the formalism of dynamical multiferroicity to the case of domain wall motion and present numerical results for the prototypical ferroelectric barium titanate (BaTiO3), based on a combination of density functional theory calculations and phenomenological modeling. We propose two experimental setups that possibly allow the detection of the dynamical magnetic field using nitrogen-vacancy center magnetometry, and we show that the magnitude of the effect lies well above the present detection limit.
 Paruch, Giamarchi, and Triscone, Topics Appl. Phys. 105, 339 (2007)
 Salje, Phase Transit. 86, 2 (2013)
 Juraschek, Fechner, Balatsky, and Spaldin, Phys. Rev. Mat. 1, 014401 (2017)
 Dunnett, Zhu, Spaldin, Juricic, and Balatsky, Phys. Rev. Lett. 122, 057208 (2019)
 Juraschek and Spaldin, Phys. Rev. Mat. 3, 064405 (2019)
EL03.08: Magnetoelectrics III
Wednesday PM, December 04, 2019
Hynes, Level 1, Room 101
1:30 PM - EL03.08.01
Delta-E Effect Magnetic Field Sensors
Franz Faupel1,Benjamin Spetzler1,Sebastian Zabel1,Phillip Durdaut1,Anne Kittmann1,Cai Müller1,Julius Schmalz1,Gerhard Schmidt1,Martina Gerken1,Jeffrey McCord1,Reinhard Knöchel1,Michael Höft1,Eckhard Quandt1
Kiel University1Show Abstract
Magnetic field sensors based on the delta-E effect utilize the resonance shift of a high frequency mechanical resonator in a magnetic field, due to the change in Young’s modulus of a magnetostrictive material. Delta-E effect sensors are not affected by 1/f amplifier noise and allow broadband magnetic field measurements at low frequencies down to DC with very high dynamic range. Moreover, they are robust against microphony effects and mechanical noise. Fully integrable magnetic field sensors were achieved via replacement of magnetic by electric excitation. Since our first publication of this sensor concept in 2011 [B. Gojdka et al., Appl. Phys. Lett. 99, 223502 (2011); Nature 480, 155 (2011)], much progress has been made in understanding the complex interplay of magnetic, mechanical and electrical properties. This holds for different designs of cantilever sensors, but also for surface acoustic wave devices. Here we present a comprehensive magneto-electromechanical model that considers the interaction of magnetic, mechanical and electrical properties and show current experimental results. We discuss the delta-E effect in general and its application in diverse types of electrically excited sensors, including the most common types such as bending or bulk resonators, but also shear resonators and surface acoustic wave sensors. The model provides detailed understanding of the general limits of the sensitivity, which arise from using the delta-E effect as the sensing principle. Realistic detection limits are predicted in combination with a noise equivalent model. The simulations are validated with experimental data using different sensor designs and magnetic layers. We also discuss simultaneous operation of delta-E sensors in the delta-E mode and the direct magnetoelectric mode, e.g. for localization of the sensor.
2:00 PM - EL03.08.02
Magnetoelectric MEMS Doubly-Clamped Resonators for Vector Magnetic Field Sensing
Peter Finkel1,Margo Staruch1,Steve Bennett1,Jeff Baldwin1,Konrad Bussmann1
U.S. Naval Research Laboratory1Show Abstract
Magnetoelectric (ME) resonators are of significant interest for next generation magnetic field sensors, as the direct coupling of magnetostrictive and piezoelectric phases enables high magnetic field sensitivity with exceptionally low operational power requirements. In this work, we present silicon based ME thin film resonators with clamped-clamped boundary conditions, that are fully suspended to achieve a string mode resonance. The heterostructure is comprised of a magnetoelastic FeCo or FeCoV layer, which is coupled through strain to an AlN piezoelectric layer with high e31,fpiezoelectric coefficients. A negative or positive shift in the resonant frequency was observed for fields applied parallel and perpendicular to the length of the beam, respectively, consistent with the magnetostriction measurements and the expected magnetoelastic strain developing in the beams due clamped-clamped boundary conditions. A linear behavior in the field dependent resonant frequency when the field is perpendicular to the length is most likely due to a well-defined hard axis in this direction resulting from high shape and stress-induced anisotropy energies. Together, these results suggest that through modification of the magnetic anisotropy, the frequency shift and angular dependence can be tuned, producing highly directional structures for magnetic field sensors. Finally, the sensor performance is evaluated and benchmarked against conventional magnetic field sensors.
3:30 PM - EL03.08.03
Phase-Field Modeling of Multiferroic Heterostructures
Long-Qing Chen1,Jia Mian Hu1,2,Jianjun Wang1,Tian-Nan Yang1
The Pennsylvania State University1,University of Wisconsin–Madison2Show Abstract
Phase-field method has been applied to modeling both direct and converse magnetoelectric effects in multiferroic heterostructures including the coupled evolution of magnetic and ferroelectric domain under electric fields. This presentation will discuss our recent applications of the phase-field method to understanding the strain-mediated voltage control of magnetic skyrmions in nanoscale multiferroic heterostructures. It is shown that a nanoscale skyrmion in a magnetic disk can be repeatedly created and deleted by strain imparted from the underlying piezoelectric layer. We analyzed the strain-mediated skyrmion switching dynamics based on both phase-field simulations and analytical theorities. We will discuss the possibility of performing high-throughput phase-field simulations of magnetic switching of multiferroic heterostructures. In particular, using a combination finite-element calculations and phase-field simulations, we studied the 3D geometrical effects of Ni islands on the strain relaxation and magnetic domain structures and switching in Ni/PMN-PT nanoscale heterostructures under an external electric field. Finally, we will also discuss potential applications of a dynamical phase-field model to understanding the ultrafast dynamics of ferroic domains in multiferroics.
4:00 PM - EL03.08.04
Strain-Mediated Magnetoelectric Effect in Self-Assembled Epitaxial Nanocomposites
Dwight Viehland1,Xiao Tang1,Min Gao1,Jiefang Li1
Virginia Tech1Show Abstract
Spinel magnetostrictive cobalt ferrite (CoFe2O4, CFO) can vertically integrate nanopillars embedded in a matrix of perovskite piezoelectric bismuth ferrite (BiFeO3, BFO), self-assembling the ‘1-3’-type nanocomposites [1, 2]. These two phases exhibit a considerable magnetoelectric (ME) effect due to the coupling via strain at the interfaces . The ME effect of CFO with either rhombohedral or tetragonal BFO has been studied [4, 5].
To further increase the ME coefficient, such ‘1-3’-type nanocomposites were epitaxially deposited on piezoelectric single crystal substrates (i.e. Pb(Mg1/3Nb2/3)O3-x%PbTiO3, PMN-xPT). An applied electric field (E) of 3 kV/cm was able to induce a giant magnetization change (~93% for ΔM/Mr), equivalent to a converse ME coefficient of 1.3×10-7 s/m . Moreover, multiple distinguishable magnetization states were obtained, which were stable on removal of the E . This multi-state ME nanocomposite thus has potential for neuromorphic-like computing and multilevel-cell memory devices.
From an energy-saving perspective, CuFe2O4 (CuFO) that shows low loss and high mechanical quality factor was used to replace the typical CFO in our ME nanocomposites . The CuFO-BFO/PMN-PT nanocomposites exhibited notably slimmer M-H loops than CFO-BFO/PMN-PT ones, and a significantly larger ME coupling effect than pure CuFO/PMN-PT heterostructures [7, 8]. The findings demonstrate a trade-off between ME effects and energy losses that can be modified by material choices and nanocomposite topography.
Our investigations on CFO-BFO and CuFO-BFO shed light on the feasibility to approach non-volatility in nanocomposites, even though the individual phases/substrate had only volatile properties . It simplifies materials selection for multi-state systems, averting difficulties with compositional non-uniformity and property repeatability in particular with regards to PMN-xPT crystal substrates.
 L. Yan, Y. Yang, Z. Wang, Z. Xing, J. Li, D. Viehland, Review of magnetoelectric perovskite–spinel self-assembled nano-composite thin films, Journal of Materials Science, 44 (2009) 5080-5094.
 J.L. MacManus-Driscoll, P. Zerrer, H. Wang, H. Yang, J. Yoon, A. Fouchet, R. Yu, M.G. Blamire, Q. Jia, Strain control and spontaneous phase ordering in vertical nanocomposite heteroepitaxial thin films, Nature Materials, 7 (2008) 314.
 Z. Wang, Y. Li, R. Viswan, B. Hu, V.G. Harris, J. Li, D. Viehland, Engineered Magnetic Shape Anisotropy in BiFeO3–CoFe2O4 Self-Assembled Thin Films, ACS Nano, 7 (2013) 3447-3456.
 M. Gao, R. Viswan, X. Tang, C.M. Leung, J. Li, D. Viehland, Magnetoelectricity of CoFe2O4 and tetragonal phase BiFeO3 nanocomposites prepared by pulsed laser deposition, Scientific Reports, 8 (2018) 323.
4:30 PM - EL03.08.05
Anisotropic Spin-Orbit Torque Generation in Epitaxial SrIrO3 by Symmetry Design
Tianxiang Nan1,2,Trevor Anderson1,Jonathan Gibbons2,Kyusung Hwang3,Neil Campbell1,Hua Zhou4,Yongqi Dong4,Gy Kim5,Dingfu Shao6,Tula Paudel6,Neal Reynolds2,Xinjun Wang7,Nian Sun7,Evgeny Tsymbal6,Siyoung Choi5,Mark Rzchowski1,Yong Baek Kim3,Daniel Ralph2,Chang-Beom Eom1
University of Wisconsin Madison1,Cornell University2,University of Toronto3,Argonne National Laboratory4,POSTECH5,University of Nebraska6,Northeastern University7Show Abstract
Spin-orbit coupling (SOC), the interaction between the electron spin and the orbital angular momentum, can unlock rich phenomena at interfaces, in particular interconverting spin and charge currents. Conventional heavy metals have been extensively explored due to their strong SOC of conduction electrons. However, spin-orbit effects in classes of materials such as epitaxial 5d-electron transition metal complex oxides, which also host strong SOC, remain largely unreported. In addition to strong SOC, these complex oxides can also provide the additional tuning knob of epitaxy to control the electronic structure and the engineering of spin-to-charge conversion by crystalline symmetry. Here, we demonstrate room-temperature generation of spin-orbit torque on a ferromagnet with extremely high efficiency via the spin-Hall effect in epitaxial metastable perovskite SrIrO3. We first predict a large intrinsic spin-Hall conductivity in orthorhombic bulk SrIrO3 arising from the Berry curvature in the electronic band structure. By manipulating the intricate interplay between SOC and crystalline symmetry, we control the spin-Hall torque ratio by engineering the tilt of the corner-sharing oxygen octahedra in perovskite SrIrO3 through epitaxial strain. This allows the presence of an anisotropic spin-Hall effect due to a characteristic structural anisotropy in SrIrO3 with orthorhombic symmetry. Our experimental findings demonstrate the heteroepitaxial symmetry design approach to engineer spin-orbit effects. We therefore anticipate that these epitaxial 5d transition-metal oxide thin films can be an ideal building block for low-power spintronics.
Nian Sun, Northeastern University
Jane Chang, University of California, Los Angeles
Shashank Priya, The Pennsylvania State University
Eckhard Quandt, University of Kiel
EL03.09: Multiferroics IV
Thursday AM, December 05, 2019
Hynes, Level 1, Room 101
8:30 AM - *EL03.09.01
Theoretical Design of Low Dimensional Polar Materials
Southeast University1Show Abstract
Achieving novel physical properties, such as superconductivity, ferromagnetism, and ferroelectricity, in two-dimensional (2D) materials should enable numerous functionalities in nanoscale devices. In recent years, interests in high-performance 2D ferroelectric materials have also grown rapidly across multiple scientific and engineering disciplines. Here, two new 2D polar materials are predicted based on physical analysis and by using density functional theory calculations. The first one is a 2D type-II multiferroic magnetoelectric material (MXene Hf2VC2F2) and and the second one is a noncollinear ferrielectricity materials (dioxydihalides MO2X2 family, where M= Mo and W; X= Cl and Br).
For multiferroic MXene Hf2VC2F2 monolayer, its ferroelectricity originates directly from its magnetism . The noncollinear 120o Y-type spin order generates a polarization perpendicular to the spin helical plane. Remarkably, the multiferroic transition is estimated to occur above room temperature.
For dioxydihalides MO2X2 monolayer, it is predicted to display noncollinear ferrielectricity, induced by competing ferroelectric and antiferroelectric soft modes . More importantly, this intrinsic noncollinearity of dipoles generates unique physical properties, such as Z2×Z2 topological domains, atomic-scale dipole vortices/anti-vortices, and negative piezoelectricity.
Our studies will open the door to a new branch of 2D materials in the pursuit of intrinsically strong magnetoelectricity and noncollinear ferrielectricity.
 J. J. Zhang, L. F. Lin, Y. Zhang, M. Wu, B. I. Yakobson, S. Dong, J. Am. Chem. Soc. 140 (2018) 9768-9773.
 L. F. Lin, Y. Zhang, A. Moreo, E. Dagotto, S. Dong, under review.
9:00 AM - *EL03.09.02
Strong Magnetoelectric Coupling by Tailoring Interfacial Chemistry and Physics in Correlated Oxides
Beijing Normal University1Show Abstract
Magnetoelectric effects, magnetic-field-mediated polarization and/or electric-field-controllable magnetism, have attracted enormous attentions owing to the growing demands of new-generation information technologies. However, large direct and/or converse magnetoelectric coupling in thin-film materials is challenging (Nat. Mater. 18, 203 (2019)), which inhibits the practical application in future high-density and high-throughput electronic/spintronic devices. Here, via artificially design of correlated oxides at atomic scale, large magnetoelectric response by controlling the interfacial chemistry and physics has been achieved, accompanying the strong interplay of spin, charge, orbital and lattice degrees of freedom. This atomic tailoring of the quantum order parameters in oxide interfaces provides an alternative pathway towards realizing strong and controllable magnetoelectric effects with thin-film integrations.
9:30 AM - EL03.09.03
Search for Local Magneto-Electric Effects in Cr2O3
Martin Dehn1,2,J. Kane Shenton3,Donald Arseneau4,Sarah Dunsiger4,Bassam Hitti4,Stefan Holenstein5,Michael Fechner6,Hubertus Luetkens7,W Andrew MacFarlane1,Ryan McFadden1,Quintin Meier3,Gerald Morris4,Zaher Salman7,Nicola Spaldin3,Robert Kiefl1,2
University of British Columbia1,Stewart Blusson Quantum Matter Institute2,ETH Zürich3,TRIUMF4,Universität Zürich5,Max Planck Institute for the Structure and Dynamics of Matter6,Paul Scherrer Institut7Show Abstract
The bulk properties of the prototypical linear magneto-electric (ME) antiferromagnet Cr2O3 have been extensively studied. Here, we report on a muon spin rotation (μSR) study using spin polarized muons to probe the local ME effect. This was motivated by the recent prediction that a point charge inside a linear ME creates a monopolar magnetic field distribution . μSR is a unique and novel way to test such predictions since the muon may act both as a test charge and a sensitive probe of the induced local magnetic field .
Prerequisite for a search for such local or muon induced magnetoelectricity is a thorough understanding of the local electronic structure and magnetic interaction of the muon within the host material. We find that the muon, a light interstitial probe, occupies several distinct stopping sites in Cr2O3, and displays a rich dynamic behavior that we interpret in the context of local muon hopping, thermally activated site transitions and the formation of a charge-neutral muon-polaron complex.
Furthermore, when Cr2O3 is prepared in a single magnetic domain, a shift in the local magnetic field is observed in response to an applied electric field, with the sign of the shift depending both on the field direction and domain state. The origin of this apparent magneto-electric effect is discussed.
 D. I. Khomskii, Nature Communications 5, 4793 (2014)
9:45 AM - EL03.09.04
Concept of Artificial Magnetoelectric Materials via Geometrically Controlling Curvilinear Helimagnets
Oleksii Volkov1,Ulrich Rößler2,Jürgen Fassbender1,Denys Makarov1
Helmholtz-Zentrum Dresden-Rossendorf e.V.1,Leibniz Institute for Solid State and Materials Research Dresden2Show Abstract
Magnetoelectric materials are of the great interest due to their unique coupling of the magnetic and electrical order parameters. In these materials magnetic states can be manipulated via electric field and vice versa, offering exciting prospectives for energy efficient memory, logic and sensor devices. However, a sizeable magnetoelectric coupling for technologically relevant applications is obtained for a limited set of single-phase bulk materials. Typically, this restriction can be removed by using two-phase materials, containing strain-coupled magnetoelectric heterostructures based on piezoelectric-magnetostrictive bilayers. Although the concept is promising, there is a clear limitation regarding the fact that strain-induced changes result in the modification of all intrinsic magnetic parameters, in particular anisotropic couplings. Ideally, it would be advantageous that electric field control of magnetic state is achieved without change of global intrinsic magnetic parameters.
We propose a novel type of artificial magnetoelectric material , which allows an electric field-induced deterministic switching between magnetic states without influencing intrinsic magnetic parameters. The proposal refers to geometrically curved helimagnets [2,3] embedded in a piezoelectric matrix or sandwiched between two piezoelectric layers. In contrast to typical strain-coupled magnetoelectric heterostructures, we exploit the geometric coupling between the piezoelectric matrix and curvilinear helimagents. Namely, a small geometrical deformation causes a drastic modification of magnetic state of the helimagnet through a magnetic phase transition between a homogeneous magnetic state and a periodical one. Resulting transformations of the average magnetization from non-zero to zero value can be uniquely assigned to logical “1” and “0”. This paves the way towards the realization of novel magnetoelectric devices with geometrically tunable and deterministically switchable magnetic states.
We provide not only the general concept but also show analytical validation for a prototypical example of torsional nanospring helimagnets. Furthermore, we put forth a discussion on the feasibility of the experimental realization of the concept including the choice of materials and fabrication approaches.
 O. M. Volkov et al., J. Phys. D: Appl. Phys. (2019). doi:10.1088/1361-6463/ab2368.
 O. M. Volkov et al., Scientific Reports 8, 866 (2018).
 R. Streubel et al., J. Phys. D: Appl. Phys. (Topical Review) 49, 363001 (2016).
10:30 AM - EL03.09.05
Contact-Free Measurement of Light-Induced Currents at Domain Walls in Multiferroic BiFeO3
Burak Guzelturk1,Antonio Mei2,Lei Zhang3,Liang Tan4,Anisha Gurcharn Singh1,Darrell Schlom2,Lane Martin3,Aaron Lindenberg1
Stanford University1,Cornell University2,University of California, Berkeley3,Lawrence Berkeley National Laboratory4Show Abstract
Multiferroic BiFeO3 (BFO) films with periodic stripe domains produce anomalously large open circuit voltages under visible light illumination with exciting promise in solar energy applications. However, the microscopic origin of this photovoltaic effect has not been understood yet. Here, we make contact-free measurements of light-induced currents in stripe domain BFO films with 71° domain walls using terahertz emission spectroscopy. With this approach, we avoid undesired modifications to the ferroelectric polarization due to the physical electrodes, hence allowing us to disentangle different photovoltaic responses intrinsic to the BFO films. Analyzing the radiated terahertz fields, we find that the current flows perpendicular to the domain walls. This observation strongly indicates the predominant role of the domain walls in the separation of photogenerated charges and enables quantitative estimates of the currents and built-in fields associated with the domain walls. Furthermore, samples with increasing domain wall density show enhanced terahertz emission providing additional evidence for domain wall-mediated charge separation. On the other hand, we find that bulk photovoltaic effects only play a minor role in the photovoltaic response of the stripe domain BFO films with a contribution smaller than 5%. This work enables new fundamental understanding of photoferroelectric responses and defines novel opportunities for ferroelectric-based optoelectronics and efficient bias-free terahertz emitters.
10:45 AM - EL03.09.06
Magnetoelectric Switching Dynamics in BiFeO3
Eric Parsonnet1,Yen-Lin Huang1,Bhagwati Prasad1,Chia-Ching Lin2,Tanay Gosavi2,Dmitri Nikonov2,Ian Young2,Vishal Ravi1,Jonathan Reichanadter1,Akshay Pattabi1,Lei Zhang1,Jeffrey Bokor1,Lane Martin1,Ramamoorthy Ramesh1
University of California, Berkeley1,Intel Corporation2Show Abstract
With room temperature coupling between magnetic and electric degrees of freedom, BiFeO3 (BFO) has attracted much attention as a leading candidate for magnetoelectric applications. These include a variety of spintronic applications such as a magnetoelectric spin orbit (MESO) logic device where there exist stringent requirements on switching speed. Although there does not exist a wealth of true time-dynamics studies of ferroelectrics, a previous study on Pb(Nb0.04Zr0.28Ti0.68)03 found ultrafast ferroelectric switching at ~220ps. Time-resolved BFO measurements have, to date, not been reported. There has been extensive work studying the equilibrium or quasi-static magnetoelectric coupling in BFO, but dynamics and fundamental limitations on switching have yet to be explored. Via pulsed ferroelectric (PUND) I-V measurements we provide novel data probing the limits of magnetoelectric switching speeds and study the effect of film thickness on dynamics. We probe the effects of chemical composition on magnetoelectric switching by studying two model systems, namely BFO and La-doped BFO. The data reveal low-nanosecond switching, much faster than previously reported in (La)BFO. Importantly, by exploring lateral scaling of device size, we demonstrate a pathway to the switching speeds required for spintronic applications. By employing giant magneto-resistance (GMR) and longitudinal magneto-optical Kerr effect (MOKE) studies, we are working towards direct observation of voltage control of magnetization on such timescales.
11:00 AM - EL03.09.07
High-Throughput Phase-Field Simulations of Anisotropy and Voltage-Controlled Magnetization in Multiferroic Heterostructures
Jianjun Wang1,Tian-Nan Yang1,Jacob Zorn1,Long-Qing Chen1
The Pennsylvania State University1Show Abstract
Understanding magnetic domain structures and their responses to electric fields in multiferroic heterostructures is critical to the design of electric-field-driven spintronic devices. In this presentation, I will show high-throughput finite-element and phase-field simulations of piezoelectric strain anisotropy and its relaxation, magnetic domain structures and their responses to applied voltages as function of the in-plane dimensions and thickness of the magnetic Ni nanoislands grown on a Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT) membrane. The piezoelectric strain anisotropy is found to increase with the in-plane aspect ratio, but it can be significantly relaxed, as large as >80%, in nanoislands of thickness larger than >15 nm. Magnetic domain diagrams are established to identify the domain structures for Ni nanoislands of different lengths of in-plane major and minor axis, as well as thickness. When a voltage is applied to the multiferroic heterostructure, the single-domain magnetic domain can be switched by the piezoelectric strain, whereas the vortex domain is not switched. However, for a multiferroic heterostructure with a thick nanoisland wherein most of the piezoelectric strain is relaxed, the single-domain magnetic domain shows a weak response to the voltage and cannot be switched by the voltage.
I will also show how to use a phase-field approach to identifying the magnetic anisotropy, which is similar to experimental rotating magneto-optical Kerr effect method and anisotropic magnetoresistance measurement, By performing high-throughput phase-field simulations to obtain thousands of M-H loops, hundreds of remanent magnetization and coercive field versus external magnetic-field direction polar diagrams can be established, which are used to further construct directional angle and coercive field of the easy axis versus strain anisotropies diagrams. Thermodynamic energy analysis are performed to understand the simulation results, which revealed that the strain anisotropy impacts the directional angle and the coercive field of the easy axis by modifying the valley and peak positions, as well as the barrier of the free energy profile. This presentation will contribute to a computational understanding of strain anisotropy and voltage-controlled magnetic properties in strain-mediated multiferroic heterostructures.
Jian-Jun Wang, Tian-Nan Yang, Jacob A. Zorn, Emily Wang, Julian Irwin, Shane Lindemann, Mark S. Rzchowski, Jia-Mian Hu, Chang-Beom Eom, Long-Qing Chen, “Strain Anisotropy and Magnetic Domain Structures in Multiferroic Heterostructures: High-throughput Finite-Element and Phase-field Studies”, Acta Materialia (2019).
11:30 AM - EL03.09.09
Control of Highly Anisotropic Ferroelastic Domains in LaCoO3 Films and Ferromagnetism Using Strain
Michael Fitzsimmons1,2,Er-Jia Guo3,2,Ryan Desautels4,2,David Keavney5,Manuel Roldan Gutierrez6,Brian Kirby7,Dongkyu Lee2,Zhaoliang Liao2,Xiang Gao2,Haile Ambaye2,Jamie Molaison2,Reinhard Boehler2,Timothy Charlton2,Andreas Herklotz8,T. Zac Ward2,Ho Lee2
University of Tennessee1,Oak Ridge National Laboratory2,Institute of Physics3,Seagate4,Argonne National Laboratory5,Arizona State University6,National Institute of Standards and Technology7,Martin-Luther-University8Show Abstract
Coupling of ferroelastic and ferromagnetic order parameters in materials offers a means to achieve novel multiferroic applications. We report the observation of one-dimensional ferroelastic domains in LaCoO3 thin films that are intimately linked to magnetization. Unidirectional structural modulation is achieved by selective choice of substrate or growth plane, which produces broken in-plane rotational symmetry. Structural modification either through film growth or application of pressure is shown to affect the magnetism. Modification perturbs the crystal field energy, which leads to unexpected in-plane anisotropy of the orbital configuration and the magnetization.
Work funded by the U.S. Department of Energy, Basic Energy Sciences
EL03.10: Magnetoelectrics IV
Thursday PM, December 05, 2019
Hynes, Level 1, Room 101
1:30 PM - EL03.10.01
Solution Processed Nanostructured Multiferroic Materials
University of California-Los Angeles1Show Abstract
In this talk, we examine multiple ways to control magnetism in solution processed nanostructured materials using an applied electrical bias. We begin with traditional multiferroic coupling, where electricity and magnetism are coupled through strain, and consider two systems. The first is a nanoporous magnetic or ferroelectric network produced using polymer templating of sol-gel oxides. The pores are then conformally filled with the opposite phase (either ferroelectric or magnetic) using atomic layer deposition to produce a three dimensional nanoscale composite. For these materials, we find the largest multiferroic response in materials with partly filled pores, emphasizing the role of residual porosity in controlling the elastic behavior and thus the multiferroic coupling of these composite materials. We next consider strain mediated switching in monolayer nanocrystal arrays. Here we show that nanocrystals can be controllably and reversibly switched from a superparamagnetic state, which has no time-averaged magnetic moment, to a ferromagnetic state using an applied bias. Finally, we explore a new type of multiferroic material, termed granular multiferroics, where exchange coupling between closely spaced magnetic nanocrystals can be modified by tuning the dielectric environment around the nanocrystals using either temperature or an applied electric field. In this work on nickel nanocrystals coupled to a soft ferroelectric, both temperature and field dependent changes in magnetism are observed in the vicinity of the ferroelectric Currie temperature, indicating that magnetism in nanocrystal arrays can indeed be tuned using dielectric changes.
2:00 PM - EL03.10.02
Voltage Control of Interfacial Magnetism in Multiferroic Based Spintronic Devices
Ming Liu1,Shishun Zhao1,Qu Yang1,Mengmeng Guan1,Zhongqiang Hu1,Ziyao Zhou1
Xi'an Jiaotong University1Show Abstract
One of the central challenges in realizing magnetoelectric (ME) devices lies in finding a deterministic way to modulate magnetism in integrated circuits with a circuit-operation voltage. Ionic liquid (IL) gating on magnetic thin films with abundant electronic, chemical and magnetic interactions at the interface has become an emerging technology for controlling magnetism in a fast, compact and energy-efficient way. Compared with conventional strain effect dominated piezo/ferroelectric layer multiferroics, IL gating method has advantages like small gating voltage (Vg<5 V), easy-to-integration and compatibility with varied substrates such as Si, flexible substrates etc. In additional, unlike the oxide structures require a high temperature to overcome the oxidation energy barrier, the IL gating control process can be operated at room temperature, suitable for applications in room temperature environment. Here, we will summarize our recent progresses of IL gating control of magnetism in varied magnetic heterostructures, as well as in dfferent manners.[1-5] As IL gating process, proven to be a truly powerful and compatible gating method, enables giant ME tunability in different heterostructures and provides a tremendous potential in next generation of voltage-tunable spintronics/electronics.
1. S. Zhao, Z. Zhou, B. Peng, M. Zhu, M. Feng, Q. Yang, Y. Yan, W. Ren, Z.G. Ye, and Y. Liu. M. Liu, Adv. Mater. 29, 1606478 (2017)
2. Q. Yang, L. Wang, Z. Zhou, S. Zhao, G. Dong, Y. Chen, T. Min, M. Liu, Nature Communication, 9, 991 (2018)
3. S. Zhao, L. Wang, Z. Zhou, C. Li, G. Dong, L. Zhang, B. Peng, T. Min, Z. Hu, J. Ma, W. Ren, Z.-G. Ye, W. Chen, P. Yu, C-W Nan, M. Liu, Adv. Mater. DOI: 10.1002/adma.201801639 (2018)
4. M. Guan, L. Wang, S. Zhao, Z. Zhou*, G. Dong, W. Su, T. Min, J. Ma, Z. Hu, W. Ren, Z.-G. Ye, C.-W. Nan, M. Liu, Adv. Mater. DOI: 10.1002/adma.201802902 (2018)
5. Q. Yang, Z. Zhou, L. Wang, H. Zhang, Y. Cheng, Z. Hu, B. Peng, and M. Liu, Adv. Mater., 30, 1800449, (2018)
2:30 PM - EL03.10.03
Investigation of Diverse Magnetic Materials via Acoustically Driven Ferromagnetic Resonance
Michael Page1,Piyush Shah2,Derek Bas1,Vladimir Safonov1,Maksym Popov3,Alexei Matyushov4,Anne Kittmann5,Viktor Schell5,Eckhard Quandt5,Ivan Lisenkov6,Gopalan Srinivasan7,Nian Sun4,Michael McConney1
Air Force Research Laboratory1,Apex Microdevices2,Taras Shevchenko National University of Kyiv3,Northeastern University4,Kiel University5,Winchester Technologies6,Oakland University7Show Abstract
Recently, magnetoelastic coupling has been exploited to detect ferromagnetic resonance (FMR) using surface acoustic waves (SAWs)1, a technique known as ADFMR. GHz-frequency SAWs are produced and detected electrically using pairs of interdigital transducers (IDTs). A magnetic material is placed in the path of the SAWs, which can then interact with magnetic moments via magnetoelastic coupling. Absorption of the SAWs occurs at FMR, modulating the measured output. Landau-Lifshitz-Gilbert theory describes the interaction in terms of the external magnetic field with a characteristic four-lobe pattern, from which the magnetic anisotropy field, FMR resonance field, and magnetoelastic coupling coefficient can be inferred.
We study the effects of a variety of magnetic materials including Ni, FeCo, FeGaB, and FeCoSiB, to examine the dependence of ADFMR patterns on material parameters and geometries. We use a range of SAW frequencies from ~300 to 2000 MHz to explore spectral effects of the IDT design on transduction efficiency, and the frequency dependence of the resonance field. We also calculate the FMR linewidth and quality factor- figures of merit useful for determining the efficacy of future ADFMR devices.
1Weiler, M. et al. (2011). Elastically driven ferromagnetic resonance in nickel thin films. Phys. Rev. Lett., 106(11), 117601.
2:45 PM - EL03.10.04
Love Wave Magnetic Field Sensors
Viktor Schell1,Phillip Durdaut1,Cai Müller1,Anne Kittmann1,Jeffrey McCord1,Michael Höft1,Eckhard Quandt1
Kiel University1Show Abstract
For the measurement of bio-magnetic signals there are high demands on the performance of the respectively utilized sensors. The requirements for these specific applications are a limit of detection (LOD) of significantly below 100 pT/Hz-1/2, a frequency bandwidth of 1 Hz to at least 20 Hz, better 100 Hz or above and a reduced size for achieving high spatial resolution or for the case of limited installation space. Further the device should be operable at room temperature and without magnetic shielding.
Promising candidates for fulfilling all these requirements are surface acoustic wave (SAW) magnetic field sensors, especially those using shear horizontal SAWs1. These so-called Love waves result from a piezoelectric substrate generating shear horizontal waves capped with a guiding layer with lower acoustic impedance confining the acoustic wave at the surface. As the sensitive element in these devices amorphous magnetostrictive thin films such as the alloy (Fe90Co10)78Si12B10 seem to be particularly promising due to their high magnetostriction with simultaneously having a low magnetic anisotropy. Operating in a delay line configuration the magnetoelastically-induced change of shear modulus of the sensitive layer (ΔE/ΔG-effect) yields in a corresponding phase shift of the acoustic wave. While the application of amorphous magnetostrictive thin films in magnetoelectric cantilever composites was already studied extensively, the sensitivity and noise behavior in SAW sensors is not quite understood yet. However the quartz based Love wave devices with a working frequency of approximately 150 MHz show already very high sensitivities of up to 2000 °/mT and an equivalent LOD of 70 pT/Hz-1/2 at 10 Hz and 30 pT/Hz-1/2 at 100 Hz.
 A. Kittmann, P. Durdaut, S. Zabel, J. Reermann, J. Schmalz, B. Spetzler, D. Meyners, N. X. Sun, J. McCord, M. Gerken, G. Schmidt, M. Höft, R. Knöchel, F. Faupel, and E. Quandt, “Wide Band Low Noise Love Wave Magnetic Field Sensor System,” Scientific Reports, vol. 8, no. 1, pp. 278–287, 2018.
This work was funded by the German Research Foundation (DFG) through the Collaborative Research Centre CRC 1261 “Magnetoelectric Sensors – From Composite Materials to Biomagnetic Diagnostics”.
3:30 PM - EL03.10.05
picoTesla Magnetoelectric Sensors with Low-Curvature Nano-Plate Resonators
Alexei Matyushov1,James Zhou2,Zhenyun Qian1,Mohsen Zaeimbashi1,Menghui Li1,Cheng Tu1,Huaihao Chen1,Yingxue Guo1,Matteo Rinaldi1,Nian Sun1
Northeastern University1,The University of Chicago2Show Abstract
Prior studies have shown the effectiveness of piezoelectric/magnetostrictive MEMS magnetometers featuring a nano plate resonator and using the ΔE effect for highly sensitive detection of DC magnetic fields. By monitoring changes in resonance frequency from applied magnetic fields, a sensitivity of a few Hz/nT has been achieved in unshielded lab environments. With dimensions of ≤ 200 μm across, and < 1 μm thick, these devices offer the advantages of small scale, including portability and low power consumption, as well as high spatial resolution in sensor arrays. However, a thorough understanding of magnetic properties and other performance aspects in these magnetometers has not been developed. In this study we report on the strong effects of resonator plate curvature on sensor performance. It was found that the total resonance frequency shift dropped off exponentially with increasing curvature by as much as two orders of magnitude. By fabricating a ΔE effect magnetometer with low curvature in the nano plate resonator, we achieved maximum magnetic field sensitivity of 4.98 Hz/nT. This is as much as two orders of magnitude higher frequency sensitivity than in other recently reported magnetometers, that also utilize the delta E effect, but which are composed of a cantilever structure and generally operate at lower frequencies.
3:45 PM - EL03.10.06
Cantilever Beam Magnetometer for Electric Field Induced Magnetization Measurements
Alliance University1,IIT Kharagpur2Show Abstract
Optical double cantilever beam magnetometer was designed, fabricated and demonstrated its ability to measure magnetostriction (in-plane and out-of-plane), magnetization and magnetocrystalline anisotropy of ferromagnetic thin films as a function of the magnetic field. Notably, for the first time, here we demonstrate the well-established and simple cantilever beam technique for electric field modification of magnetization of ferromagnetic/ferroelectric heterostructures by considering the induced strains in ferromagnetic thin films through the converse piezoelectric effect in piezoelectric films. Moreover, this set-up also allows measuring the electromechanical properties such as transversal piezoelectric strain (d31) and stress (e31) coefficients of piezoelectric thin films. This magnetometer is simple in construction, inexpensive to manufacture, easy to operate along with noise subtraction provision and having sensitivity nearly 8 nm in the determination of cantilever beam deflection.
4:00 PM - EL03.10.07
Magnetoelectric Composite Sensor Based on Magnetostrictive Multilayers for Magnetic Frequency Conversion
Lars Thormählen1,Matic Jovičević Klug1,Sebastian Toxværd1,Michael Höft1,Eckhard Quandt1,Jeffrey McCord1,Dirk Meyners1
Faculty of Engineering CAU Kiel1Show Abstract
Magnetoelectric composites have been studied intensively in the recent past because of their preeminent magnetoelectric coupling, opening the path to highly sensitive magnetic field sensors operating at room temperature . Moreover, this sensor approach yields the advantage to optimize the constituting phases independently. In the context of magnetic field sensing, the role of the magnetostrictive component is to respond to an external magnetic field by generating mechanical stress onto the piezoelectric phase. At least as important, irregular magnetization changes resulting from hysteretic effects have to be avoided in order to prevent significant noise contribution to the sensor output . The multilayer approach increases the parameter space, which can be used to jointly attune the magnetoelastic response towards high sensitivity and improved control of magnetization reversal .
The presented work focuses on thin film magnetostrictive phase composites, composed of (Fe90Co10)78Si12B10 multilayers. These layers are based on the stacking order unit Ta 5 / Cu 3 / MnIr 8 / FeCoSiB x [thickness in nm] with varying the FeCoSiB layer thickness x. The total thickness of the FeCoSiB layers is adjusted to 1 µm, 2 µm and 4 µm. The piezoelectric component is a 2 µm thick AlN layer. The constituents are grown on a Si substrate, one each side, by RF and pulsed DC sputter deposition respectively. Using UV lithography combined with dry and wet etching, magnetoelectric cantilever structures are fabricated with typical lateral dimensions of 2.3 mm x 25 mm. Applying a multistep thermal treatment, parallel and antiparallel alignment of magnetizations in adjacent ferromagnetic layers is achieved in order to formulate a stable domain configuration in the magnetic layers .
The presentation reports on recent advances achieved by utilizing magnetostrictors that are exchange biased layer by layer. Applying magnetic frequency conversion yields minimum detectable magnetic fields as low as 50 pT/ Hz1/2 at 10 Hz , demonstrating the significantly improved performance of such macroscopic magnetoelectric field sensors.
Funding of the project work by the German Research Foundation through the CRC 1261 Magnetoelectric Sensors: From Composite Materials to Biomagnetic Diagnostics is gratefully acknowledged.
 Leung, C. M. et al.: A review on applications of magnetoelectric composites: from heterostructural uncooled magnetic sensors, energy harvesters to highly efficient power converters, J. Phys. D 51 (2018), 263002.
 Urs, N. O. et al.: Origin of hysteretic magnetoelastic behavior in magnetoelectric 2-2 composites, Appl. Phys. Lett. 105 (2014), 202406
 Röbisch, V. et al.: Pushing the detection limit of thin film magnetoelectric heterostructures, J. Mater. Res. 32 (2017), 1009.
 M. Jovičević Klug, L. Thormählen et al.: Antiparallel exchange biased multilayers for low magnetic noise magnetic field sensors, Appl. Phys. Lett. 114 (2019), 192410.
 Salzer, S. et al.: Noise Limits in Thin-Film Magnetoelectric Sensors with Magnetic Frequency Conversion, IEEE Sensors Journal, 18, (2018) no. 2, pp. 596-604.
4:15 PM - EL03.10.08
TiNiCu Thin-Film Shape Memory Alloy Substrates for Tunable Resonant Frequency Magnetoelectric Sensors
Sabrina Curtis1,2,Duygu Dengiz1,Hanna Lewitz1,Lars Thormählen1,Justin Jetter1,Dirk Meyners1,Eckhard Quandt1
Kiel University1,University of Maryland2Show Abstract
Magnetic field sensors based on magnetoelectric composites can offer powerful diagnosis of biomagnetic signals originating in the brain and torso. Thin-film magnetoelectric (ME) composites comprised of FeCoSiB as the magnetostrictive layer and AlN as the piezoelectric layer have demonstrated sensors with a high sensitivity and low limit of detection at biomagnetic relevant frequencies. A magnetoelectric sensor will have its highest sensitivity when operated at its mechanical resonant frequency. Some medical operations, such as deep brain stimulation, would require a ME sensor with a tunable resonant frequency to locate the stimulated area of the brain during operation. This is a major limitation as most state-of-the-art ME sensors are mechanically designed to operate at one single resonant frequency. In this work, we show introducing a functionalized shape memory alloy (SMA) layer to the ME composite can offer a tunable ME sensor through a reversible gradual change in the Young’s modulus (E) of SMA material.
Here, AlN / FeCoSiB thin-film magnetoelectric composites are fabricated and characterized on functional TiNiCu SMA substrates. Through an induced temperature pulse, it is possible to gradually change the Young’s modulus of the SMA, thereby changing the mechanical resonant frequency of the magnetoelectric sensor . Our analytical calculations show that the resonant frequency can be altered by 6% for a magnetoelectric sensor (2 µm AlN / 2 µm FeCoSiB / 25 µm TiNiCu / 100 µm Si) through a temperature induced reversible solid-to-solid phase transformation of the SMA from martensite (E = 41 GPa) to austenite (E = 83 GPa). For a 2.5 mm x 20 mm cantilever the resonant frequency can be gradually increased from 318 Hz to 340 Hz purely through this transformation. The difference in frequency between martensite and austenite phases becomes enhanced by increasing TiNiCu film thickness, or by eliminating the Si substrate.
Currently, MEMS compatible fabrication routes are being explored to build a full magnetoelectric sensor onto a TiNiCu substrate for experimentally verification. Characterization results on the effect of heat treatment and TiNiCu surface roughness on the growth and material performance of the piezoelectric layer (AlN) through piezoforce microscopy (PFM), X-ray diffraction (XRD), double beam laser interferometry (DBLI) and transmission electron microscopy (TEM) will be presented.
Funding from the DFG is greatly acknowledged for this work
 Röbisch, Volker, et al. "Frequency-tunable nickel-titanium substrates for magnetoelectric sensors." AIP Advances 8.12 (2018): 1253
4:30 PM - EL03.10.09
400MHz MEMS Antenna Based on Magnetoelectric Coupling Effect
Huaihao Chen1,Xianfeng Liang1,Neville Sun1,Hwaider Lin2,Yuan Gao2,Nian Sun1,2
Northeastern University1,Winchester Technology, LLC2Show Abstract
400MHz frequency band is the most commonly used band for Medical Implant Communications Service (MICS). However, most of recent antenna researches for this application are based on electromagnetic wave resonance, which lead to a comparable size to the wavelength [1, 2]. To solve this problem, a new antenna design based on the magnetoelectric coupling is introduced by our group , which is a thin-film bulk acoustic resonance (FBAR) antenna for 2.5GHz applications, based on the AlN resonator and magnetoelectric coupling. Since acoustic wave has smaller wavelength than electromagnetic wave, the antenna size can be easily scaled down by more than 100 times. However, for most AlN resonator designs, impedance matching is a problem because of the high electric impedance. Hence, a parallel antenna array structure is applied to reduce the impedance and increase the antenna gain .
In this work, nano-plate resonance (NPR) antenna arrays for 400MHz application are designed, fabricated and tested. This antenna is based on the magnetoelectric coupling between AlN thin film and FeGaB/SiO2 multilayer. The antenna array structure is shown in Fig. 1 (a) with 8um width and array numbers of 1,4, 8 and 16. This strip structure resonates at in-plane mode, and this resonance is limited in width direction by the strip. The measured S-parameters are shown in Fig. 1 (b), with operating frequency of 371MHz, and 10dB-bandwidth of 3.875MHz. A radiation peak of S21 is observed clearly at the resonant frequency, and a peak antenna gain of -54.82dBi is achieved. This radiation peak is from the vibration and domain rotation of magnetic film. The measured S11 and calculated Z11 are shown in Fig. 2. For fewer array numbers, the impedance is higher, and the related return loss is also higher, so the radiation peak is cover by the baseline. For this reason, array structure with more than 16 strips is necessary for impedance matching and high antenna gain.
 C. Liu, Y.-X. Guo, and S. Xiao, "Compact dual-band antenna for implantable devices," IEEE Antennas and Wireless Propagation Letters, vol. 11, pp. 1508-1511, 2012.
 N. Cho, T. Roh, J. Bae, and H.-J. Yoo, "A planar MICS band antenna combined with a body channel communication electrode for body sensor network," IEEE Transactions on Microwave Theory and Techniques, vol. 57, no. 10, pp. 2515-2522, 2009.
 T. Nan et al., "Acoustically actuated ultra-compact NEMS magnetoelectric antennas," Nature communications, vol. 8, no. 1, p. 296, 2017.
 R. Gardelli, M. Albani, and F. Capolino, "Array thinning by using antennas in a Fabry–Perot cavity for gain enhancement," IEEE Transactions on Antennas and Propagation, vol. 54, no. 7, pp. 1979-1990, 2006.
4:45 PM - EL03.10.10
Electric Field Control of Magnetism in Double Perovskites Coupled with Bismuth Ferrite
Vishal Ravi1,Bhagwati Prasad1,Yen-Lin Huang1,Jose Flores2,Fengyuan Yang2,Ramamoorthy Ramesh1
University of California, Berkeley1,The Ohio State University2Show Abstract
Multiferroic materials offer exciting pathways to manipulate both magnetic and electronic properties simultaneously, which, in the case of bismuth ferrite, stem from the intrinsic linking of ferroelectric and antiferromagnetic degrees of freedom. By leveraging this fundamental coupling, we can modify and indeed switch the ferromagnetism of materials such as Co0.9Fe0.1 that sit adjacent to ferroelectric bismuth ferrite thin films, using only electric fields . Using an oxide ferromagnet instead, such as La0.7Sr0.3MnO3, could potentially confer on these devices an improved fatigue life, as oxidation may be less critical .
This electric field control of magnetism through magnetic coupling opens up a vast array of applications, particularly in logic, data, and spintronics, where we may manipulate magnetic memories such as magnetic tunnel junctions with the application of an electric field, instead of through more energy-intensive spin-transfer torque currents .
Double perovskites, such as Sr2FeMoO6 (SFMO) and Sr2CrReO6 (SCRO), are promising candidates for ferromagnets that may provide such coupling with bismuth ferrite. As half-metallic oxides with Curie points higher than room temperature, both materials exhibit spin-polarised currents and potential perpendicular magnetic anisotropy, which are desirable for magnetic tunnel junctions and other magnetoresistance-based devices . Additionally, as these films are oxides rather than pure metals, they could provide an interface that is more robust against oxidation, leading to longer fatigue life.
We show the enhancement of these double perovskites’ coercive fields atop bismuth ferrite when compared to their isolated phases, which could uncover clues as to the strength of any magnetic coupling at the interface. We also explore magnetoelectric coupling by studying the effects of electric fields on the magnetisation of these double perovskites on bismuth ferrite, through giant magnetoresistance and anisotropic magnetoresistance measurements, in addition to correlated magnetic force microscopy and piezoresponse force microscopy images. These materials could lead to the next generation of low-power data storage and logic device technology.
 Heron, J. T., Trassin, M., Ashraf, K., Gajek, M., He, Q., Yang, S. Y., … Ramesh, R. (2011). Electric-field-induced magnetization reversal in a ferromagnet-multiferroic heterostructure. Physical Review Letters, 107(21). https://doi.org/10.1103/PhysRevLett.107.217202
 Wu, S. M., Cybart, S. A., Yu, P., Rossell, M. D., Zhang, J. X., Ramesh, R., & Dynes, R. C. (2010). Reversible electric control of exchange bias in a multiferroic field-effect device. Nature Materials, 9(9), 756–761. https://doi.org/10.1038/nmat2803
 Amiri, P. K., Alzate, J. G., Cai, X. Q., Ebrahimi, F., Hu, Q., Wong, K., … Wang, K. L. (2015). Electric-Field-Controlled Magnetoelectric RAM: Progress, Challenges, and Scaling. IEEE Transactions on Magnetics, 51(11). https://doi.org/10.1109/TMAG.2015.2443124
 Meetei, O. N., Erten, O., Mukherjee, A., Randeria, M., Trivedi, N., & Woodward, P. (2013). Theory of half-metallic double perovskites. I. Double exchange mechanism. Physical Review B - Condensed Matter and Materials Physics, 87(16). https://doi.org/10.1103/PhysRevB.87.165104
 Vaitheeswaran, G., Kanchana, V., & Delin, A. (2006). Electronic structure of the ferromagnetic double-perovskites Sr 2CrReO6, Sr2CrWO6, and Ba 2FeReO6. Journal of Physics: Conference Series, 29(1), 50–53. https://doi.org/10.1088/1742-6596/29/1/008 Amiri, P. K., Alzate, J. G., Cai, X. Q., Ebrahimi, F., Hu, Q., Wong, K., … Wang, K. L. (2015). Electric-Field-Controlled Magnetoelectric RAM: Progress, Challenges, and Scaling. IEEE Transactions on Magnetics, 51(11). https://doi.org/10.1109/TMAG.2015.2443124
Nian Sun, Northeastern University
Jane Chang, University of California, Los Angeles
Shashank Priya, The Pennsylvania State University
Eckhard Quandt, University of Kiel
EL03.11: Multiferroics V
Friday AM, December 06, 2019
Hynes, Level 1, Room 101
8:30 AM - EL03.11.01
Nanoscale Field Dependencies of Domain Wall Configurations in 3D Revealed by Tomographic Atomic Force Microscopy
Bryan Huey1,Jingfeng Song1,Thomas Moran1,Michael Martin1,James Steffes1,Aiping Chen2,Ramamoorthy Ramesh3
University of Connecticut1,Los Alamos National Laboratory2,University of California, Berkeley3Show Abstract
Magnetoelectric sensing and efficiency in multiferroics is a function of ferroelectric domain dynamics. Understanding domain configurations at various stages in the switching process can therefore reveal switching mechanisms, a necessary step in ultimately optimizing system performance and efficiency. However, these can be strongly influenced by often experimentally inaccessible sub-surface effects, including thickness dependencies, microstructural or compositional heterogeneities, interfaces, and depending on the device design even simple geometric influences. Therefore, we recently introduced Tomographic-AFM for direct volumetric materials property mapping. 3-D resolved domain configurations and thickness dependent switching are specifically reported for monolithic La doped BiFeO3, and a BiFeO3/CoFeO3 vertically aligned nanocomposite. In each case, ferroelectric domain nucleation and growth are further investigated as a function of thickness. Pure BiFeO3 clearly obeys Kay-Dunn thickness scaling and a multistep switching process, and such multistep 180° switching is also observed for the La doped and nanocomposite films despite the substantially different local microstructure and even composition. Reconfigurations of domain walls upon electric field annealing furthermore lend insight into domain and domain wall stabilities.
9:00 AM - EL03.11.02
Functionally Active Domain Walls in Ferroics and Multiferroics
Queen's Univ Belfast1Show Abstract
It is now well established that ferroelectric and multiferroic domain walls often have unique functional properties that are completely different from the domains that they surround: they can be semiconducting, metallic and even superconducting when the rest of the material is insulating; they can display magnetic order, which is absent elsewhere, and can possess aligned electrical dipoles when the matrix surrounding them is non-polar. In effect, ferroelectric and multiferroic domain walls represent a new class of nanoscale functional material. Crucially, they can be controllably shunted from point to point, created, or made to disappear; hence, a completely new paradigm of transient nanoscale devices may be possible, based on a “now-you-see-it, now-you-don’t” dynamic deployment of domain walls.
This talk will explore progress towards the realisation of these kinds of dreams and in particular show how injection, movement and removal of domain walls have enabled active control of nanoscale thermal conduction (in LaAlO3 and LiNbO3), the appearance of local negative capacitance (in Cu-Cl boracites), the existence of 1D mobile p-n junctions (in ErMnO3 and Cu-Cl boracites) and the design of a new form of domain-wall memristor (in LiNbO3).
9:30 AM - EL03.11.03
Design and Fabrication of ZnO-Based SMR Magnetoelectric Antennas for High-Gain Applications
Xianfeng Liang1,Huaihao Chen1,Neville Sun1,Yuan Gao2,Hwaider Lin2,Nian Sun1
Northeastern University1,Winchester Technologies, LLC2Show Abstract
Magnetoelectric (ME) antennas based on the suspended ME circular disk consisting of FeGaB/AlN thin-film have been demonstrated recently . However, the FBAR devices are very fragile and delicate due to the releasing structure, although the complicated packaging process  is able to solve this problem. From the device point of view, the solid mounted resonator (SMR) with Bragg reflector has attracted much attention as a promising technology for the film bulk acoustic wave resonator (FBAR) devices . Typically, the SMR devices are formed of a piezoelectric film, such as ZnO that is sandwiched between top and bottom metal electrodes, on top of a Bragg reflector. A resonance is created when a radio frequency (RF) signal is applied across the FBAR device. There are a variety of products such as filters , duplexers , and voltage controlled oscillators (VCOs)  based on SMR designs have been developed in past years.
In this work, we designed, fabricated and tested ZnO-based SMR ME antennas that operate at GHz with high gain performance. As shown in Fig. 1, the Bragg reflector consisting of three pairs of SiO2/W layers was sputter deposited in one run with RF reactive magnetron sputtering for SiO2 and DC sputtering for W. The piezoelectric ZnO layer was sputter deposited by RF reactive sputtering with Zn target and high-purity Oxygen gas. The XRD curves and rocking curves for ZnO films under different temperature were measured and exhibited in Fig. 2. In order to grow high quality ZnO films, it is vital to have sufficient ion bombardment during deposition. Therefore, high temperature of 450 degrees Celsius is preferred here with rocking curve FWHM of 2.25 degrees. After optimizing the performance of Bragg reflector and piezoelectric ZnO films, we fabricated and tested the SMR ME antennas. A gain enhancement of 12 dB was achieved in this novel design for robust ME antennas. Therefore, it is very promising in practical applications.
 T. Nan, H. Lin, Y. Gao, A. Matyushov, G. Yu, H. Chen, et al., "Acoustically actuated ultra-compact NEMS magnetoelectric antennas," Nature communications, vol. 8, p. 296, 2017.
 J. D. Larson III, S. Ellis, and Y. Oshmyansky, "Film bulk acoustic resonator (fbar) devices with simplified packaging," ed: Google Patents, 2008.
 R. Ruby, "11E-2 Review and comparison of bulk acoustic wave FBAR, SMR Technology," in 2007 IEEE Ultrasonics Symposium Proceedings, 2007, pp. 1029-1040.
 R. Ruby, P. Bradley, D. Clark, D. Feld, T. Jamneala, and K. Wang, "Acoustic FBAR for filters, duplexers and front end modules," in 2004 IEEE MTT-S International Microwave Symposium Digest (IEEE Cat. No. 04CH37535), 2004, pp. 931-934.
 R. Boudot, M. Li, V. Giordano, N. Rolland, P. Rolland, and P. Vincent, "A solid-mounted resonator-oscillator-based 4.596 GHz frequency synthesis," Review of Scientific Instruments, vol. 82, p. 034706, 2011.
9:45 AM - EL03.11.04
Design and Fabrication of Miniature Magnetoelectric Antennas Using a Solidly Mounted Resonator Structure
Neville Sun1,Yuan (Daniel) Gao2,Mohan Sanghadasa3,Nian Sun1
Northeastern University1,Winchester Technologies, LLC2,U.S. Army Combat Capabilities Development Command Aviation & Missile Center3Show Abstract
One of the key challenges to state-of-the-art antennas lies in their size miniaturization. Conventional antennas rely on an EM wave resonance and require a size of more than one tenth of the EM wavelength λ0. In this work, a new miniature magnetoelectric (ME) antenna is presented utilizing the multilayer Bragg reflector structure of a solidly mounted resonator (SMR) to enhance small scale antenna gain up to -16 dBi. The antenna radiates using a magnetoelectric heterostructure consisting of AlN and FeGaB with resonator diameters of 500 um and 1000 um. Different ME resonator shapes and sizes are designed, fabricated and compared along with varying anchor widths and lengths to provide better impedance matching. The acoustic resonance in the heterostructure films operates with an out-of-plane mode of vibration so that the thickness of each layer was optimized to produce a resonant frequency at 1.5 and 2.45 GHz to allow for seamless on-chip integration with WiFi, Bluetooth and GPS devices. The SMR structure replaces the freestanding membrane structure  with a Bragg acoustic reflector for concentrated energy confinement. The Bragg reflector was fabricated with a quarter wavelength mode configuration to create maximum particle displacement in the AlN and FeGaB layers. Three periods of alternating low and high acoustic impedance films, using silicon dioxide and tungsten respectively, were deposited on top of a silicon substrate to provide greater acoustic resonance within the ME heterostructure. Antenna gain measurements were performed in an anechoic chamber using a GSG probe and a reference horn antenna linked to a vector network analyzer. The robust features of the SMR has more advantages compared to its FBAR freestanding membrane counterpart allowing for low cost monolithic integration, high operating frequency, better thermal dissipation and structural stability that will be vital for small-scale antennas and other wireless applications.
 T. Nan, H. Lin, Y. Gao, A. Matyushov, G. Yu, H. Chen, et al., "Acoustically actuated ultra-compact NEMS magnetoelectric antennas," Nature communications, vol. 8, p. 296, 2017.
10:30 AM - EL03.11.05
Epitaxially Engineered, Enhanced Magnetostriction in Strain-Driven Composite Multiferroic
Peter Meisenheimer1,Rachel Steinhardt2,Shihao Zhuang3,Suk Hyun Sung1,Mark Nowakowski4,Steve Novakov1,Bhagwati Prasad4,Chris Zollner2,Zhe Wang2,Natalie Dawley2,Allen Hunter1,Sasi Manipatruni5,Dmitri Nikonov5,Ian Young5,Long-Qing Chen6,Jeffrey Bokor4,Ramamoorthy Ramesh4,Robert Hovden1,Jia Mian Hu3,Darrell Schlom2,John Heron1
University of Michigan1,Cornell University2,University of Wisconsin–Madison3,University of California, Berkeley4,Intel Corporation5,The Pennsylvania State University6Show Abstract
Composite multiferroics, composed of a magnetostrictive ferromagnet and a piezoelectric ferroelectric, have widely been targeted for beyond-CMOS logic due to their large coupling coefficients and high operating temperature1–3. Magnetoelectric multiferroic systems potentially offer the lowest energy dissipation per bit operation in a scalable platform, yet significant materials challenges still exist in the field. For composite multiferroics, this requires finding pathways to enhance piezomagnetic effects and coupling between layers, an effort that has seen relatively little work4. Here, we present a means to boost the magnetostriction of Fe1-xGax alloys and magnetoelectric coupling in a Fe1-xGax - (PMN-PT) composite multiferroic heterostructure through epitaxy.
In bulk, the magnetostriction coefficient of Fe1–xGax alloys versus Ga composition peaks near ~18% Ga occurring due to a phase change from the disordered A2 phase to an ordered BCC phase (D03), which reduces the magnetostriction coefficient5. A distinct advantage of thin film deposition is the potential to access metastable phases through epitaxy, allowing us to promote the chemically disordered BCC (A2) phase in our film at high (22%) Ga concentrations. We demonstrate that thin film epitaxy stabilizes a chemically disordered BCC Fe0.78Ga0.22 alloy where the magnetostriction is enhanced by 200-300% relative to the bulk.
Transport-based magnetoelectric characterization shows 90 electrical switch of magnetic anisotropy and one of the largest converse magnetoelectric coefficients ever achieved at room temperature in a composite multiferroic[jH1] and energy dissipation per operation scaling to 5.9 J cm-2, making our devices competitive with other state-of-the-art beyond CMOS technologies6. This hyperactive performance is achieved through epitaxial stabilization of a disordered, metastable phase of earth-abundant and rare-earth-free magnetostrictor, Fe0.78Ga0.22. By epitaxially engineering our ferromagnetic layer to prevent the formation of deleterious intermetallic nanoregions, we provide a pathway to engineering new performance levels in rare-earth free magnetoelastic and magnetoelectric heterostuructures.
1. Meisenheimer, P. B., Novakov, S., Vu, N. M. & Heron, J. T. Perspective: Magnetoelectric switching in thin film multiferroic heterostructures. J. Appl. Phys. 123, 240901 (2018).
2. Ramesh, R. & Spaldin, N. A. Multiferroics: progress and prospects in thin films. Nat. Mater. 6, 21–29 (2007).
3. Bibes, M. & Barthélémy, A. Multiferroics: Towards a magnetoelectric memory. Nat. Mater. 7, 425–426 (2008).
4. Shevlin, S. Multiferroics and the path to the market. Nat. Mater. 18, 191 (2019).
5. Du, Y. et al. Relation between Ga ordering and magnetostriction of Fe-Ga alloys studied by x-ray diffuse scattering. Phys. Rev. B 81, 054432 (2010).
6. Manipatruni, S. et al. Scalable energy-efficient magnetoelectric spin–orbit logic. Nature 565, 35–42 (2019).
10:45 AM - EL03.11.06
Room Temperature Lead Zirconium Palladium Titanate Multiferroic Nanoscale Films
Karuna Mishra1,Alvaro Instan1,Mohan Bhattarai1,Ram Katiyar1
University of Puerto Rico1Show Abstract
Growth of single-phase magnetoelectric materials and their analysis of coupling mechanisms between ferroic order parameters (spin and polarization) is important from the point of view of next generation logic and memory devices. Herein, we report fabrication, dielectric, ferroelectric and magnetic measurement of a Pd-doped room-temperature magnetoelectric multiferroic Pb(Zr0.20Ti0.80)0.70Pd0.30O3-δ (PZTPd) thin film. Highly oriented PZTPd thin films were deposited on (LaAlO3)0.3(Sr2AlTaO6)0.7 substrates by following laser ablation processes in oxygen atmosphere using pulsed laser deposition technique. X-rays diffraction studies revealed that the film had tetragonal phase with c-axis orientation. The surface morphology studies using atomic force and scanning electron microscopic techniques suggest a smooth and homogeneous distribution of grains on the surface of the film with roughness ~1.8 nm. Temperature dependent dielectric measurements were carried out in Pt/ PZTPd /LSMO metal-ferroelectric-metal capacitors that showed diffused behavior over a large range of temperatures at several frequencies, and exhibited a higher dielectric constant ~3000 at 100 Hz at room temperature. The polarization hysteresis loops were obtained at room temperature, attributed to its ferroelectric behavior. Piezo force microscopy suggests a random polarization orientation in a grown film, whereas polarizations could be switched easily with a positive and negative electric bias. A well-saturated magnetization M-H loop with remanent magnetization of 1.6 emu/cm3 was observed at room temperature. The reason for magnetization in PZTPd thin film is found to be due to mixed oxidation states of Pd2+/Pd4+ in the Pb(Zr0.20Ti0.80)O3 matrix as complemented by x-rays photoelectron spectroscopic results. These findings suggest that our thin films are multiferroic (ferroelectric-ferromagnetic) at room temperature. The details will be presented in the meeting.
11:00 AM - EL03.11.07
Hydrogen-Driven Switching of Magnetic Anisotropy—Insights from First-Principles
Konstantin Klyukin1,Geoffrey Beach1,Bilge Yildiz1,2
Massachusetts Institute of Technology1,Department of Nuclear Science and Engineering2Show Abstract
Resistive and magnetic switching phenomena have recently attracted large interest for ultra-scaled non-volatile memory and logic devices. The incorporation of hydrogen can significantly influence magnetic and electronic properties of functional materials allowing effective tuning magnetic anisotropy, magnetic moment and electroresistance. Despite extensive experimental investigations, very little is known about the phenomena on a molecular level and systematic investigations are needed to provide fundamental insights on the physical origin of phenomena. In this work, we consider a series of heterostructures (Co/Pd, MgO/Fe, etc) exhibiting perpendicular magnetic anisotropy (PMA) and employ density functional theory calculations (DFT) to determine the critical concentration of hydrogen needed for magnetic anisotropy switching. We show that anisotropy switching effect is mainly attributed to the electronic structure changes at the interface, while lattice expansion caused by hydrogen insertion plays a minor role. These results clarify the underlying mechanisms of magnetic anisotropy switching and help optimizing material combinations for hydrogen-based magneto-ionic devices.
11:15 AM - EL03.11.08
First-Principles Prediction of Muon Stopping Sites in Magnetoelectric Cr2O3
J. Kane Shenton4,Martin Dehn1,2,Stefan Holenstein3,Quintin Meier4,Donald Arseneau2,Sarah Dunsiger2,Bassam Hitti2,Hubertus Luetkens3,W Andrew MacFarlane2,1,Ryan McFadden1,Gerald Morris2,Zaher Salman3,Nicola Spaldin4,Michael Fechner5,4,Robert Kiefl1,2
University of British Columbia1,TRIUMF2,Paul Scherrer Institut3,ETH Zurich4,Max Planck Institute for the Structure and Dynamics of Matter5Show Abstract
Recent conceptual advances in our understanding of magnetoelectrics have led to renewed interest in materials such as Cr2O3. Muon spin rotation (µSR) is a promising technique for investigating recently predicted local magnetoelectric phenomena, acting as a probe of the local magnetic field at the muon stopping site(s). The ab initio prediction of muon stopping sites in materials is crucial to correctly interpreting µSR experiments. However, the quantum nature of the muon, together with its short lifetime (~2.2 µs), allow the muon to exhibit a rich range of dynamical phenomena that are challenging to capture using standard first-principles methods. Furthermore, the impact of the positively charged muon on the surrounding lattice can lead to significant changes to the muon behaviour and experienced local field.
Here we report on a µSR study of Cr2O3, focussing on the theoretical prediction of muon stopping sites and dynamics. We find that quantum corrections beyond the harmonic approximation are required to obtain accurate energy barriers between muon stopping sites. We also find strong evidence for a charge-neutral muon-polaron complex in Cr2O3, stabilised by a Jahn-Teller distortion. The latter finding has important implications for the charge state and behaviour of hydrogen defects in Cr2O3 and related materials.