Spin-Flip Optical Excitations in van der Waals Antiferromagnet CrPS<sub>4</sub>.

Jana, Dipankar; Soll, Aljoscha; Sofer, Zdenek; Orlita, Milan; Faugeras, Clement; Koperski, Maciej; Potemski, Marek · Nano Lett · 2026

basic_science · Level V

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Abstract

We investigate the near-infrared optical response of the semiconducting van der Waals antiferromagnet CrPS<sub>4</sub> 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 CrPS<sub>4</sub>. From the magnetic field evolution of the optical transition, we extract key magnetic parameters, including the spin-flop (<math xmlns="http://www.w3.org/1998/Math/MathML"><mo>≈</mo><mn>0.9</mn></math> T) and spin-saturation (<math xmlns="http://www.w3.org/1998/Math/MathML"><mo>≈</mo><mn>8</mn></math> 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.