Unravelling Photoinduced Interlayer Spin Transfer Dynamics in Two-Dimensional Nonmagnetic-Ferromagnetic van der Waals Heterostructures

Although light is the fastest means to manipulate the interfacial spin injection and magnetic proximity related quantum properties of two-dimensional (2D) magnetic van der Waals (vdW) heterostructures, its potential remains mostly untapped. Here, inspired by the recent discovery of 2D ferromagnets Fe3GeTe2 (FGT), we applied the real-time density functional theory (rt-TDDFT) to study photoinduced interlayer spin transfer dynamics in 2D nonmagnetic-ferromagnetic (NM-FM) vdW heterostructures, including graphene-FGT, silicene-FGT, germanene-FGT, antimonene-FGT and h-BN-FGT interfaces. We observed that laser pulses induce significant large spin injection from FGT to nonmagnetic (NM) layers within a few femtoseconds. In addition, we identified an interfacial atom-mediated spin transfer pathway in heterostructures in which the photoexcited spin of Fe first transfers to intralayered Te atoms and then hops to interlayered NM layers. Interlayer hopping is approximately two times slower than intralayer spin transfer. Our results provide the microscopic understanding for optically control interlayer spin dynamics in 2D magnetic heterostructures.

Automated summary

This study utilized real-time density functional theory to investigate the photoinduced interlayer spin transfer dynamics in two-dimensional nonmagnetic-ferromagnetic van der Waals heterostructures, leading to the observation of significant spin injection induced by laser pulses. Additionally, an atom-mediated spin transfer pathway was identified, shedding light on the microscopic understanding of optically controlling interlayer spin dynamics in 2D magnetic heterostructures.