Ultrafast Laser Control of Antiferromagnetic–Ferrimagnetic Switching in Two-Dimensional Ferromagnetic Semiconductor Heterostructures

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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 CrCl 3 /CrBr 3 heterostructures with antiparallel (AP) and parallel (P) systems. Although an ultrafast demagnetization of CrCl 3 and CrBr 3 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.