Realizing ultrafast control of magnetization switching is of crucial importance for information processing and recording technology. Here, we explore the laser-induced spin electron excitation and relaxation dynamics processes of CrCl3/CrBr3 heterostructures with antiparallel (AP) and parallel (P) systems. Although an ultrafast demagnetization of CrCl3 and CrBr3 layers occurs in both AP and P systems, the overall magnetic order of the heterostructure remains unchanged due to the laser-induced equivalent interlayer spin electron excitation. More crucially, the interlayer magnetic order switches from antiferromagnetic (AFM) to ferrimagnetic (FiM) in the AP system once the laser pulse disappears. The microscopic mechanism underpinning this magnetization switching is dominated by the asymmetrical interlayer charge transfer combined with a spin-flip, which breaks the interlayer AFM symmetry and ultimately results in an inequivalent shift in the moment between two FM layers. Our study opens up a new idea for ultrafast laser control of magnetization switching in two-dimensional opto-spintronic devices.

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

Department of Physics University of Science and Technology of China Hefei Anhui 230026 China

Departments of Chemistry and Physics and Astronomy University of Southern California Los Angeles California 90089 United States

School of Physics Southeast University Nanjing 211189 China

School of Science Constructor University Bremen 28759 Germany

Shenzhen JL Computational Science and Applied Research Institute Shenzhen 518109 China

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