Ultrashort laser pulses are extensively used for efficient manipulation of interfacial spin injection in two-dimensional van der Waals (vdW) heterostructures. However, physical processes accompanying the photoinduced spin transfer dynamics on the all-semiconductor ferromagnetic vdW heterostructure remain largely unexplored. Here, we present a computational investigation of the femtosecond laser pulse induced purely electron-mediated spin transfer dynamics at a time scale of less than 50 fs in a vdW heterostructure. The latter is composed of two semiconducting monolayers, namely, a ferromagnetic material CrSBr and a nonmagnetic phosphorene, and is denoted as CrSBr-P. We observe an ultrafast spin injection from the Cr atoms to the P atoms in a few femtoseconds by both optically induced and interfacial atom-mediated spin transfer effects. We also show that the demagnetization and spin transfer in the ferromagnetic-nonmagnetic CrSBr-P vdW heterostructure can be sensitively manipulated by laser pulses with different fluences. Our study offers a microscopic understanding of spin dynamics in these vdW heterostructures aiming toward their potential spintronic applications, which rely on optically controlled spin transfer processes.

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

Eastern Institute for Advanced Study Eastern Institute of Technology Ningbo Zhejiang 315200 China

Institute for Advanced Study Chengdu University Chengdu 610106 China

School of Physics State Key Laboratory of Electronic Thin Films and Integrated Devices University of Electronic Science and Technology of China Chengdu 611731 China

School of Science Constructor University Bremen 28759 Germany

Theoretical Division Center for Nonlinear Studies and Center for Integrated Nanotechnologies Los Alamos National Laboratory Los Alamos New Mexico 87545 United States

Yangtze Delta Region Institute University of Electronic Science and Technology of China Huzhou 313001 China

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