Photoinduced Spin Injection and Ferromagnetism in 2D Group III Monochalcogenides

Strong light-matter interactions in low-dimensional materials offer an opportunity for flexible property-tuning by optical switching. Herein, we exploit photoexcitation for spin injection into semiconductors by rationally designing heterojunctions having distinct dynamic behavior for photocarriers in two spin channels. As a proof-of-concept, we trigger homogeneous magnetism in a group III monochalcogenide monolayer (MX with M = In, Ga; X = S, Se) by placing it on a ferromagnetic CrI₃ substrate under light illumination. Our time-dependent ab initio nonadiabatic molecular dynamics simulations reveal fast electron-hole separation for the majority spin channel but rapid recombination for the minority spin channel at this heterostructure. The majority carriers cause hole doping and strong ferromagnetic ordering in the MX sheet, with magnetic moment tunable by the injected carriers' concentration. The interplay between photoexcited hole carriers, the Van Hove singularity of MX monolayers, and interfacial charge transfer provides essential physical insights for nondestructively manipulating charge and spin in two-dimensional semiconductors via light switching.