On the Ordering Mechanism of Cu+ in 2D van der Waals Multiferroic CuCrP2S6

Guo, Jiasen; Cheng, Yongqiang; Susner, Michael A.; Siebenaller, Ryan P.; Morgan, Zachary; Ye, Feng

doi:10.1002/advs.202524227

Title: On the Ordering Mechanism of Cu⁺ in 2D van der Waals Multiferroic CuCrP₂S₆

Journal Article · Wed Feb 04 00:00:00 UTC 2026 · Advanced Science

DOI: https://doi.org/10.1002/advs.202524227 · OSTI ID:3030363

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Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Air Force Research Laboratory (AFRL), Wright-Patterson AFB, OH (United States)
The Ohio State Univ., Columbus, OH (United States)

CuCrP₂S₆ is a van der Waals multiferroic where the tunable Cu⁺ sublattice underpins its exceptional ferroelectric and electronic switching properties. Yet, the microscopic mechanism governing Cu⁺ ordering has remained elusive. Here, we combine single-crystal X-ray and neutron diffraction with pair distribution function analysis to uncover a temperature-driven evolution of Cu⁺ ordering, giving rise to an incommensurate quasi-antipolar phase between the paraelectric and antiferroelectric states. The modulation originates from correlated Cu⁺ occupancy redistribution coupled to breathing distortion of surrounding S₃ triangles, establishing a symmetry-adapted lattice distortion mode. Diffuse scattering persisting over 35 K above the transition confirms that the structural instability follows an order-disorder mechanism. The spontaneous off-centering of Cu⁺ positions CuCrP₂S₆ as a model platform for correlated order-disorder phenomena in 2D layered ferroics, and provides design principles for next-generation memory and logic devices.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Semiconductor Technology Center (NSTC); US Air Force Office of Scientific Research (AFOSR); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 3030363

Journal Information:: Advanced Science, Journal Name: Advanced Science Journal Issue: 21 Vol. 13; ISSN 2198-3844

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: On the Ordering Mechanism of Cu+ in 2D van der Waals Multiferroic CuCrP2S6

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Title: On the Ordering Mechanism of Cu⁺ in 2D van der Waals Multiferroic CuCrP₂S₆