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Manipulating spin in antiferromagnetic (AFM) materials has great potential inAFM opto-spintronics. Laser pulses can induce a transient ferromagnetic (FM)state in AFM metallic systems, but have never been proven in two-dimensional(2D) AFM semiconductors and related van der Waals (vdW) heterostructures. Here,using 2D vdW heterostructures of FM MnS2 and AFM MXenes as prototypes, weinvestigated optically induced interlayer spin transfer dynamics based on thereal-time time-dependent density functional theory (rt-TDDFT). We observed thatlaser pulses induce significant spin injection and the interfacialatom-mediated spin transfer from MnS2 to Cr2CCl2. In particular, we firstdemonstrated the transient FM state in semiconducting AFM/FM heterostructuresduring photoexcited processes. Because the proximity magnetism breaks themagnetic symmetry of Cr2CCl2 in heterostructures. Our results provide themicroscopic understanding for optically controlled interlayer spin dynamics in2D magnetic heterostructures and open a new way to manipulate magnetic ordersin ultrafast opto-spintronics.

Ultrafast optically induced magnetic state transition in 2D antiferromagnets