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DOE OSTI · 3020018

Spin-lattice entanglement in CoPS 3

Mai, Thuc T. [National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States); Air Force Research Laboratory, Wright-Patterson Air Force Base, OH (United States); Bluehalo, LLC, Dayton, OH (United States)] (ORCID:0000000200628821)·McCreary, Amber [National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)]·Garrity, K. F. [National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000302634157)·Dally, Rebecca L. [National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000165892802)·Shah, Sambridhi [University of Tennessee, Knoxville, TN (United States)] (ORCID:0000000250681735)·Chakoumakos, Bryan C. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000278706543)·Taj, Md Nasim Afroj [University of Virginia, Charlottesville, VA (United States)] (ORCID:0000000295426746)·Lynn, Jeffrey W. [National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000336264932)·McGuire, Michael A. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000317629406)·Conner, Benjamin S. [Air Force Research Laboratory, Wright-Patterson Air Force Base, OH (United States); Azimuth Corporation, Fairborn, OH (United States)]·Zebarjadi, Mona [University of Virginia, Charlottesville, VA (United States)]·Musfeldt, Janice L. [University of Tennessee, Knoxville, TN (United States)]·Hight Walker, Angela R. [National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)]·Rao, Rahul [Air Force Research Laboratory, Wright-Patterson Air Force Base, OH (United States)] (ORCID:0000000264150185)·Susner, Michael A. [Air Force Research Laboratory, Wright-Patterson Air Force Base, OH (United States)] (ORCID:0000000212118749)
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Abstract

Complex chalcogenides in the 𝑀⁢PS 3 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 CoPS 3 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 𝑇 Néel . Lastly, these findings point to strong spin-phonon entanglement as well as opportunities to control these effects under external stimuli.

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MagnetismMagnonsSpin-orbit couplingSpin-phonon couplingVan der Waals systems

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Mai, Thuc T. [National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States); Air Force Research Laboratory, Wright-Patterson Air Force Base, OH (United States); Bluehalo, LLC, Dayton, OH (United States)] (ORCID:0000000200628821), McCreary, Amber [National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)], Garrity, K. F. [National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000302634157), Dally, Rebecca L. [National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000165892802), Shah, Sambridhi [University of Tennessee, Knoxville, TN (United States)] (ORCID:0000000250681735), Chakoumakos, Bryan C. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000278706543), Taj, Md Nasim Afroj [University of Virginia, Charlottesville, VA (United States)] (ORCID:0000000295426746), Lynn, Jeffrey W. [National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000336264932), McGuire, Michael A. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000317629406), Conner, Benjamin S. [Air Force Research Laboratory, Wright-Patterson Air Force Base, OH (United States); Azimuth Corporation, Fairborn, OH (United States)], Zebarjadi, Mona [University of Virginia, Charlottesville, VA (United States)], Musfeldt, Janice L. [University of Tennessee, Knoxville, TN (United States)], Hight Walker, Angela R. [National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)], Rao, Rahul [Air Force Research Laboratory, Wright-Patterson Air Force Base, OH (United States)] (ORCID:0000000264150185), Susner, Michael A. [Air Force Research Laboratory, Wright-Patterson Air Force Base, OH (United States)] (ORCID:0000000212118749). 2025-12-16. Spin-lattice entanglement in CoPS 3. https://doi.org/10.1103/nbp7-glqj

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