Raman Fingerprints of Phase Transitions and Ferroic Couplings in van der Waals Multiferroic CuCrP₂S₆.

Authors

Jing Tang, Benjamin J Lawrie, Mouyang Cheng, Yueh-Chun Wu, Huan Zhao, Dejia Kong, Ruiqi Lu, Ching-Hsiang Yao, Zheng Gai, An-Ping Li, Mingda Li, Xi Ling

Published in

The journal of physical chemistry letters. Pages 4336-4345. Apr 23, 2025. Epub Apr 23, 2025.

Abstract

CuCrP₂S₆ (CCPS), a type-II multiferroic material, exhibits unique phase transitions involving ferroelectric, antiferroelectric, and antiferromagnetic ordering. In this study, we conduct a comprehensive investigation on the intricate phase transitions and their multiferroic couplings in CCPS across a wide temperature range from 4 to 345 K through Raman spectroscopic measurements down to 5 cm^-1. We first assign the observed Raman modes with the support of theoretical calculations and angle-resolved polarized Raman measurements. We further present clear signatures of phase transitions from the analyses of temperature-dependent Raman spectral parameters. Particularly, two low-frequency soft modes are observed at 36.1 cm^-1 and 70.5 cm^-1 below 145 K, indicating the antiferroelectric to quasi-antiferroelectric transition. Moreover, phonon mode hardening is observed when the temperature increases from 4 to 65 K, suggesting negative thermal expansion (NTE) and strong magnetoelastic coupling below 65 K. These findings advance the understanding of vdW multiferroic CCPS, paving the way for future design and engineering of multiferroicity in cutting-edge technologies, such as spintronics and quantum devices.

PMID:
40267361
Bibliographic data and abstract were imported from PubMed on 24 Apr 2025.

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