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Correlation between exciton dynamics and spin structure in the van der Waals antiferromagnet NiPS3

Kang Wang1,*,†, Yingchen Peng1,*, Boying Huang2,*, Chun Zhou3, Qianlu Sun4, Fujie Tang2,‡, Weigao Xu4, Kezhao Du5, Xingzhi Wang3 et al.

Ye Yang1,§

  • 1The State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), College of Chemistry & Chemical Engineering, Xiamen University, Xiamen 361005, China
  • 2Pen-Tung Sah Institute of Micro-Nano Science and Technology, Xiamen University, Xiamen 361005, Fujian Province, China
  • 3Department of Physics, Xiamen University, Xiamen 361005, China
  • 4Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
  • 5Fujian Provincial Key Laboratory of Advanced Materials Oriented Chemical Engineering, Fujian Normal University, Fuzhou 350007, People's Republic of China

  • *These author contributed equally to this work.
  • †Present address: Strait Institute of Flexible Electronics (SIFE, Future Technologies), Fujian Key Laboratory of Flexible Electronics, Fujian Normal University and Strait Laboratory of Flexible Electronics (SLoFE), Fuzhou, Fujian 350117, People's Republic of China.
  • ‡Contact author: tangfujie@xmu.edu.cn
  • §Contact author: ye.yang@xmu.edu.cn

Phys. Rev. B 112, L220413 – Published 26 December, 2025

DOI: https://doi.org/10.1103/nl4q-ghdg

Abstract

The emerging magnetic van der Waals (vdW) materials provide a platform for exploring novel physics regarding magnetism in low dimensions and developing ultrathin spintronic applications. Here, we investigate the ultrafast dynamics of excitons in a vdW NiPS3 crystal. The temporal evolution of the transient reflection spectra indicates that the spin-correlated exciton is formed through photocarrier localization, the rate of which is independent of the magnetic degrees of freedom. However, the recombination rate of these excitons correlates with the long-range magnetic order, likely arising from a spin-flip rooted in the underlying antiferromagnetic background during the recombination. Our findings uncover intertwined coupling between carrier, lattice, and spin degrees of freedom in NiPS3, which may pave the path toward ultrafast optical manipulation of spin-related quantum states in vdW antiferromagnets.

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