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Impact of magnons, defects, and rapid energy migration on the optical properties of the 2D magnet CrPS4

Jacob T. Baillie1, Eden Tzanetopoulos1, Rachel T. Smith1, Rémi Beaulac2, and Daniel R. Gamelin1,*

  • *Contact author: gamelin@uw.edu
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Phys. Rev. Materials 10, 054001 – Published 1 May, 2026

DOI: https://doi.org/10.1103/wmmx-thx3

Abstract

Strong coupling between optical and magnetic excitations could enable contactless, spatially resolved, or ultrafast interrogation and control of magnetism in two-dimensional (2D) materials and devices. The layered 2D A-type antiferromagnet CrPS4 stands out among van der Waals (vdW) magnets for its rich optical fine structure, but its spectroscopy is not yet understood and has so far been interpreted without consideration of magnetic exchange. Here, we show that this fine structure comes primarily from exchange-mediated coupling between on-site optical “spin-flip” transitions of Cr3+ and low-energy spin transitions involving the surrounding lattice. Well-resolved magnon sidebands to optical A24↔E2 transitions are observed in photoluminescence (PL) and PL excitation spectra, as well as a pronounced PL sideband associated with short-range exchange splitting. Energy migration is probed using Yb3+ dopants as traps, revealing subpicosecond intersite excitation hopping. Formation of dispersive Frenkel excitons of coupled on-site d-d transitions because of intersite exchange is discussed. In addition to impacting how optical fine structure is interpreted in this and potentially other vdW magnets, these findings may have ramifications for future applications of layered 2D magnets by suggesting potential routes to drive mode-specific spin-wave excitations using light.

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Phys. Rev. Materials 10, 054001– Published 1 May, 2026
  • Received 9 December 2025
  • Accepted 27 March 2026
Article part of CHORUS
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