Unveiling the spin evolution in van der Waals antiferromagnets via magneto-exciton effects

Xingzhi Wang (), Qishuo Tan, Tie Li, Zhengguang Lu, Jun Cao, Yanan Ge, Lili Zhao, Jing Tang, Hikari Kitadai, Mingda Guo, Yun-Mei Li, Weigao Xu, Ran Cheng, Dmitry Smirnov and Xi Ling ()
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Xingzhi Wang: Xiamen University
Qishuo Tan: Boston University
Tie Li: Xiamen University
Zhengguang Lu: National High Magnetic Field Laboratory
Jun Cao: Boston University
Yanan Ge: Xiamen University
Lili Zhao: Nanjing University
Jing Tang: Boston University
Hikari Kitadai: Boston University
Mingda Guo: University of California
Yun-Mei Li: Xiamen University
Weigao Xu: Nanjing University
Ran Cheng: University of California
Dmitry Smirnov: National High Magnetic Field Laboratory
Xi Ling: Boston University

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Among the fascinating phenomena observed in two-dimensional (2D) magnets, the magneto-exciton effect stands out as a pivotal link between optics and magnetism. Although the excitonic effect has been revealed and exhibits a considerable correlation with the spin structures in certain 2D magnets, the underlying mechanism of the magneto-exciton effect remains underexplored, especially under high magnetic fields. Here we perform a systematic investigation of the spin-exciton coupling in 2D antiferromagnetic NiPS3 under high magnetic fields. When an in-plane magnetic field is applied, the exceptional sharp excitonic emission at ~1.4756 eV exhibits a Zeeman-like splitting with g ≈ 2.0, experimentally identifying the exciton as an excitation of dominant triplet-singlet character. By examining the polarization of excitonic emission and simulating the spin evolution, we further verify the correlation between excitonic emission and Néel vector in NiPS3. Our work elucidates the mechanism behind the spin-exciton coupling in NiPS3 and establishes a strategy for optically probing the spin evolutions in 2D magnets.

Date: 2024
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DOI: 10.1038/s41467-024-51643-9

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