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Microscopic NMR evidence for successive antiferroelectric and antiferromagnetic order in the van der Waals magnet CuCrP2S6

C. S. Saramgi1,2, L. F. Prager1, S. Selter1, Y. Shemerliuk1,2, S. Aswartham1,3, B. Büchner1,2,4, H.-J. Grafe1,*, and K. M. Ranjith1,4,5,†

  • *Contact author: h.grafe@ifw-dresden.de
  • †Contact author: ranjith.km1857@gmail.com
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Phys. Rev. B 114, 034413 – Published 10 July, 2026

DOI: https://doi.org/10.1103/ggvw-rh72

Abstract

We present a comprehensive P31 and Cu65 nuclear magnetic resonance (NMR) study of the layered van der Waals magnet CuCrP2S6. The compound exhibits a sequence of structural and magnetic phase transitions: a high-temperature paraelectric state, followed by a quasiantiferroelectric (QAFE) state near 185 K, a long-range antiferroelectric (AFE) phase below 150 K, and finally, antiferromagnetic (AFM) order below TN = 30 K. The evolution of the NMR spectra, NMR shift, and spin-lattice (T1−1) and spin-spin (T2−1) relaxation rates provide direct microscopic fingerprints of these transitions. The splitting of both the NMR line and T1−1 below the AFE transition demonstrates the emergence of two inequivalent P sites. From K−χ analysis, we extract nearly isotropic transferred hyperfine couplings and show that the NMR shift anisotropy originates primarily from the dipolar contribution, in contrast to Mn2P2S6 and Ni2P2S6. We determine the ferromagnetic intralayer exchange Jintra≈−4.9 K from the Curie-Weiss temperature, consistent with ferromagnetic layers antiferromagnetically stacked along the c axis, and evaluate the Moriya high-temperature relaxation rate including cross-correlation effects of the P–P dimer. Critical divergence of T1−1 near TN yields a critical exponent γ≃ 0.45(4), placing CuCrP2S6 in a three-dimensional Heisenberg universality regime.

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Phys. Rev. B 114, 034413– Published 10 July, 2026
  • Received 20 January 2026
  • Revised 2 April 2026
  • Accepted 9 June 2026
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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