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 derWaals 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.
| Original language | English |
|---|---|
| Pages (from-to) | 2144351-21443510 |
| Number of pages | 19299160 |
| Journal | Physical Review B |
| Volume | 112 |
| Issue number | 21 |
| DOIs | |
| State | Published - Dec 16 2025 |
Funding
Work at the University of Tennessee (S.S. and J.L.M.) is supported by the Physical Behavior of Materials, Basic Energy Sciences, U.S. Department of Energy (Contract No. DE-SC0023144). Work at the University of Virginia (M.Z. and M.N.A.T.) is supported by the National Science Foundation under Grant No. 2421213. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Work at Oak Ridge National Laboratory was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. The work at AFRL is supported by the Air Force Office of Scientific Research (AFOSR) Grant No. LRIR 23RXCOR003. Work at the University of Tennessee (S.S. and J.L.M.) is supported by the Physical Behavior of Materials, Basic Energy Sciences, U.S. Department of Energy (Contract No. DE-SC0023144). Work at the University of Virginia (M.Z. and M.N.A.T.) is supported by the National Science Foundation under Grant No. 2421213. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Work at Oak Ridge National Laboratory was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. The work at AFRL is supported by the Air Force Office of Scientific Research (AFOSR) Grant No. LRIR 23RXCOR003. Certain trade names and company products are identified in order to adequately specify the experimental procedure. In no case does such identification imply recommendation or endorsement by the National Institute of Standards and Technology, nor does it imply that the products are necessarily the best for the purpose.