Modeling Spin-Control by Ferroelectric Switching

A key advantage of spin-defect based quantum technologies is the potential to engineer the defect properties by modifying the atomic environment. Systems which exhibit coupling between magnetic and electric degrees of freedom provide a route to manipulate spins by applying an electric-field, suggesting the prospect of localized spin-control via electrostatic gating.<br/><br/>We have elucidated the fundamental limit of magnetoelectric coupling by electric-field control of magnetic dopants in ferroelectric hosts, demonstrating through combined first principles calculations and electron-paramagnetic resonance measurements that the spin directionality evolves following a switching path coupled to polarization switching.[1]<br/><br/>We further leverage the versatility of the ferroelectric oxide platform by modifying the crystal field environment of the defect through epitaxial strain, low symmetry hosts and emergent topological polarization textures.[2,3] Results demonstrating spin-control in these systems provide an enhanced understanding of spin-charge coupling in defect systems and offer novel routes to tailored spin-control in ferroelectric crystals.<br/><br/>[1] J. Liu, V. V. Laguta, K. Inzani, W. Huang, S. Das, R. Chatterjee, E. Sheridan, S. M. Griffin, A. Ardavan, R. Ramesh, Coherent electric field manipulation of Fe³⁺ spins in PbTiO₃. <i>Science Advances</i>, <b>7</b>, eabf8103 (2021).<br/>[2] Inzani, K., Pokhrel, N., Leclerc, N., Clemens, Z., Ramkumar, S. P., Griffin, S. M., Nowadnick, E. A. Manipulation of spin orientation via ferroelectric switching in Fe-doped Bi₂WO₆ from first principles. <i>Physical Review B</i>, <b>105</b>(5), 054434 (2022).<br/>[3] S. Das, V. V. Laguta, K. Inzani, W. Huang, J. Liu, R. Chatterjee, M. R. McCarter, S. Susarla, A. Ardavan, J. Junquera, S. M. Griffin, R. Ramesh, Inherent Spin–Polarization Coupling in a Magnetoelectric Vortex. <i>Nano Letters,</i> <b>22</b>, 3976 (2022).