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    Coupling of magnetic and lattice collective excitations in the two-dimensional van der Waals antiferromagnet FePS3

    Kartik Panda1, Itzik Kapon2, Dumitru Dumcenco2, Dirk van der Marel2, Alexey B. Kuzmenko2, and Nimrod Bachar1,*

    • *Contact author: nimib@ariel.ac.il

    Phys. Rev. B 113, 235124 – Published 15 June, 2026

    DOI: https://doi.org/10.1103/fwb8-fwjb

    Abstract

    We combine polarized infrared magnetotransmission and Faraday angle rotation measurements to map the collective excitations of the van der Waals antiferromagnet FePS3. Below the Néel temperature (TN≈118K), the phonon spectrum becomes strongly anisotropic, reflecting the underlying zigzag antiferromagnetic order. In contrast, a prominent excitation at 122cm−1 (15 meV) is polarization-independent, hardens on cooling, and splits linearly with magnetic field, identifying its magnetic origin. From absolute transmission and Faraday rotation, we reconstruct the circular optical conductivities and reveal a pronounced dichroism of the field-split excitations. The upper branch near 129cm−1 exhibits a reduced dichroic response, consistent with hybridization with a nearby infrared phonon. Several phonon modes exhibit sizable Faraday rotation, providing evidence for spin-phonon coupling and demonstrating that lattice vibrations acquire magnetic-field-dependent optical activity. In addition, additional excitations appear in the infrared spectra and a broad midinfrared feature near 900cm−1 emerges only below TN, consistent with a modified lattice response in the magnetic state. These results highlight the anisotropic nature of spin-phonon coupling in FePS3 and establish polarization-resolved magneto-optical spectroscopy as a powerful probe of coupled spin and lattice dynamics in two-dimensional antiferromagnets.

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