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Ultrafast spin dynamics and Janus-induced surface-selective spin accumulation in a NiBrCl bilayer: a real-time TDDFT
Laijin Yan1, Xinlu Cheng1, Hong Zhang2
1Institute of Atomic and Molecular Pysics, Sichuan University, Chengdu 610064, China. chengxl@scu.edu.cn.
None:
We investigate the ultrafast spin dynamics of a Janus NiBrCl bilayer under femtosecond laser excitation using real-time time-dependent density functional theory. The system exhibits pronounced nonequilibrium spin behavior within 50 fs, characterized by rapid demagnetization of both Ni sublattices and a transient breakdown of antiferromagnetic compensation. The Br atoms show spin dynamics closely following the Ni sites, indicating strong p-d hybridization and ligand-mediated spin polarization. In contrast, the Cl sublattice exhibits a strongly site-dependent response: the interfacial Cl1 atom remains nearly inactive, while the outer-surface Cl2 atom hosts a significant negative spin accumulation despite weak charge transfer and negligible conduction-band occupation. Real-space magnetization density analysis further confirms a highly anisotropic spin redistribution, revealing that ultrafast magnetic dynamics are governed by Ni-Br coherent demagnetization and Janus-induced surface-selective spin accumulation at the outer Cl layer. These results highlight the crucial role of structural asymmetry in controlling ultrafast spin transport in two-dimensional magnetic materials.
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