biostudies-literatureWang XU.S. Department of Energy (DOE)National Science Foundation (NSF)8011https://www.ebi.ac.uk/biostudies/studies/S-EPMC11399334biostudies-literatureUnknown15(1)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 exNature communicationsUnveiling the spin evolution in van der Waals antiferromagnets via magneto-exciton effects.PMC113993341945364DE-SC0021064Ling XCao JKitadai HLu ZLi YMTang JGuo MZhao LLi TGe YCheng RWang XXu WTan QSmirnov DfalseUnveiling the spin evolution in van der Waals antiferromagnets via magneto-exciton effects.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 ex2024-01-01T00:00:00Z2024 Sep2026-06-01T10:07:57.608Z2025-04-04T02:50:34.948ZS-EPMC113993343927166010.1038/s41467-024-51643-9