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Optical magneto-spectroscopy methods (Raman scattering, far-infraredtransmission, and photoluminescence) have been applied to investigate theproperties of the NiPS3 semiconducting antiferromagnet. The fundamental magnongap excitation in this van der Waals material has been found to be split intotwo components, in support of the biaxial character of the NiPS3antiferromagnet. Photoluminescence measurements in the near-infrared spectralrange show that the intriguing 1.475 eV-excitation unique to the NiPS3antiferromagnetic phase splits upon the application of the in-plane magneticfield. The observed splitting patterns are correlated with properties of magnonexcitations and reproduced with the simple model proposed. Possible routestoward a firm identification of the spin-entangled 1.475 eV-optical excitationin NiPS3, which can hardly be recognized as a coherent Zhang-Rice exciton, arediscussed.

Magnon gap excitations and spin-entangled optical transition in van der Waals antiferromagnet NiPS3