Ultrafast optical control of magnetism had great potential to revolutionize magnetic storage technology and spintronics, but for now, its potential remains mostly untapped in two-dimensional (2D) magnets. Here, using the state-of-the-art real-time time-dependent density functional theory (rt-TDDFT), we demonstrate that an ultrafast laser pulse can induce a ferromagnetic state in nonmagnetic MoSe2 monolayers interfaced with van der Waals (vdW) ferromagnetic MnSe2. Our results show that the transient ferromagnetism in MoSe2 derives from photoinduced direct ultrafast interlayer spin transfer from Mn to Mo via a vdW-coupled interface, albeit with a delay of approximately a few femtoseconds. This delay was strongly dependent on laser duration and interlayer coupling, which could be used to tune the amplitude and rate spin transfer. Furthermore, we have also shown that ferromagnetic states can be photoinduced in other transition metal dichalcogenides (TMDs), such as PtS2 and TaSe2 monolayers. Overall, our findings provide crucial physical insights for exploring light-induced interlayer spin and charge dynamics in 2D magnetic systems.

Beijing Computational Science Research Center Beijing 100193 China

Bremen Center for Computational Materials Science University of Bremen Bremen 28359 Germany

Department of Physical and Macromolecular Chemistry Faculty of Science Charles University Prague Prague 12843 Czech Republic

School of Physics University of Electronic Science and Technology of China Chengdu 610054 China

Shenzhen JL Computational Science and Applied Research Institute Shenzhen 518110 China

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