ArXiv · 2026
We investigate the near-infrared optical response of the semiconducting van der Waals antiferromagnet CrPS₄ and identify previously unreported spin-entangled optical resonances. The strong and anisotropic magnetic-field dependence of these resonances reflects the underlying magnetic order and confirms the biaxial antiferromagnetic nature of CrPS₄. From the magnetic field evolution of the optical transition, we extract key magnetic parameters, including the spin-flop (≈0.9~T) and spin-saturation (≈8~T) fields. These results demonstrate a potential pathway for all-optical probing of spin states in van der Waals antiferromagnets, with relevance for spin-sensitive optoelectronic and magneto-optical devices.
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