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Spin-lattice entanglement in CoPS3

Thuc T. Mai1,2,3,*, Amber McCreary1, K. F. Garrity4, Rebecca L. Dally5, Sambridhi Shah6, Bryan C. Chakoumakos7, Md Nasim Afroj Taj8, Jeffrey W. Lynn9, Michael A. McGuire10 et al.

Benjamin S. Conner2,11, Mona Zebarjadi12, Janice L. Musfeldt6,13, Angela R. Hight Walker1, Rahul Rao2, and Michael A. Susner2,†

  • *Contact author: thuc.mai.ctr@us.af.mil
  • †Contact author: michael.susner.1@us.af.mil

Phys. Rev. B 112, 214435 – Published 16 December, 2025

DOI: https://doi.org/10.1103/nbp7-glqj

Abstract

Complex chalcogenides in the MPS3 family of materials (M=Mn, Fe, Co, and Ni) display remarkably different phase progressions depending upon the metal center orbital filling, character of the P–P linkage, and size of the van der Waals gap. There is also a stacking pattern and spin-state difference between the “lighter” and “heavier” transition-metal-containing systems that places CoPS3 at the nexus of these activities. Despite these unique properties, this compound is underexplored. Here, we bring together Raman scattering spectroscopy and infrared absorption spectroscopy with x-ray techniques to identify a structural component to the 119 K magnetic ordering transition. With temperature-dependent Raman scattering, we discover a set of magnon-phonon pairs that engages in avoided crossings below TNéel. These findings point to strong spin-phonon entanglement as well as opportunities to control these effects under external stimuli.

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Corrections

15 January, 2026

Correction: A typographical error in the email address of the byline footnote for the last author has been fixed.

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