Dec 3, 2024
8:30am - 9:00am
Sheraton, Second Floor, Back Bay B
Maksym Kovalenko1,2
ETH Zürich1,Empa–Swiss Federal Laboratories for Materials Science and Technology2
LHP NCs are of broad interest as classical light sources (LED/LCD displays) and as quantum light sources (quantum sensing and imaging, quantum communication, optical quantum computing). The current development in LHP NC surface chemistry, using designer phospholipid capping ligands, allows for their increased stability down to single particle level [1]. The brightness of such a quantum emitter is ultimately described by Fermi’s golden rule, where a radiative rate is proportional to its oscillator strength (intrinsic emitter property) and the local density of photonic states (photonic engineering, i.e., cavity). With perovskite NCs, we present a record-low sub-100 ps radiative decay time for CsPb(Br/Cl)<sub>3</sub>, almost as short as the reported exciton coherence time, by the NC size increase to 30 nm [2]. The characteristic dependence of radiative rates on QD size, composition, and temperature suggests the formation of giant transition dipoles, as confirmed by effective-mass calculations for the case of the giant oscillator strength. Importantly, the fast radiative rate is achieved along with the single-photon emission despite the NC size being ten times larger than the exciton Bohr radius. When such bright and coherent QDs are assembled into superlattices, collective properties emerge, such as superradiant emission from the inter-NC coupling [3]. In the most recent work [4], the functionality of the second SL component can give rise to the enhancement of the LHP NCs properties or the emergence of new collective effects. We present the formation of multicomponent SLs made from the CsPbBr<sub>3</sub> NCs of two different sizes. The diversity of obtained SLs encompassed the binary ABO<sub>6</sub>-, ABO<sub>3</sub>-, and NaCl-type structures, all of which contained orientationally and positionally confined NCs. For the selected model system, the ABO<sub>6</sub>-type SL, we observed efficient NC coupling and Förster-like energy transfer from strongly confined 5.3 nm CsPbBr<sub>3</sub> NCs to weakly confined 17.6 nm CsPbBr<sub>3</sub> NCs. Exciton spatiotemporal dynamics measurements reveal that binary SLs exhibit enhanced exciton diffusivity compared to one-component SLs across the entire temperature range (from 5 K to 298 K). Observed incoherent NC coupling and controllable excitonic transport within the solid NC SLs hold promise for potential applications in optoelectronic devices.<br/><br/><br/>[1] V. Morad, A. Stelmakh, M. Svyrydenko, L.G. Feld, S.C. Boehme, M. Aebli, J. Affolter, C.J. Kaul, N.J. Schrenker, S. Bals, Y. Sahin, D.N. Dirin, I. Cherniukh, G. Raino, A. Baumketner, M.V. Kovalenko <i>Nature</i>, <b>2024</b>, 626, 542–548<br/>[2] C. Zhu, S.C. Boehme, L.G. Feld, A. Moskalenko, D.N. Dirin, R.F. Mahrt, T. Stöferle, M.I. Bodnarchuk, A.L. Efros, P.C. Sercel, M.V. Kovalenko, G. Rainò. Nature, <b>2024</b>, 626, 535–541<br/>[3] I. Cherniukh, G. Rainò, T. Stöferle, M. Burian, A. Travesset, D. Naumenko, H. Amenitsch, R. Erni, R.F. Mahrt, M.I. Bodnarchuk & M.V. Kovalenko. <i>Nature</i> <b>2021</b>, 593, 535–542<br/>[4] T.V. Sekh, I. Cherniukh, E. Kobiyama, T.J. Sheehan, A. Manoli, C. Zhu, M. Athanasiou, M. Sergides, O. Ortikova, M.D. Rossell, F. Bertolotti, A. Guagliardi, N. Masciocchi, R. Erni, A. Othonos, G. Itskos, W.A. Tisdale, T. Stöferle, G. Rainò, M.I. Bodnarchuk, and M.V. Kovalenko. <i>ACS Nano</i> <b>2024</b>, 8423–8436