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Origin of versatile polarization state in CuInP2S6

Xuanlin Zhang1,2, Chengcheng Xiao3, Zeying Zhang4, Luqi Dong2, Hui Pan5, Chao Cao2, Shengyuan A. Yang5, Su-huai Wei6, and Yunhao Lu2,1,*

  • 1State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China
  • 2School of Physics, Zhejiang University, Hangzhou 310027, China
  • 3Departments of Materials and Physics, and the Thomas Young Centre for Theory and Simulation of Materials, Imperial College London, London SW7 2AZ, United Kingdom
  • 4College of Mathematics and Physics, Beijing University of Chemical Technology, Beijing 100029, China
  • 5Institute of Applied Physics and Materials Engineering, University of Macau, Macao S. A. R., China
  • 6Beijing Computational Science Research Center, Beijing 100193, China

  • *luyh@zju.edu.cn

Phys. Rev. B 108, L161406 – Published 16 October, 2023

DOI: https://doi.org/10.1103/PhysRevB.108.L161406

Abstract

Exotic electric polarization-related phenomena have recently been reported in layered van der Waals material such as CuInP2S6 and its derivatives, but the physical origin for such behaviors, especially the formation of quadrupole-well ferroelectric states and the anomalous polarization switching between these states, has not been clearly understood. Here, we provide a simple theoretical explanation using group theory analysis, highlighting the role of local symmetry-determined orbital interactions between copper ions and surrounding ligands. Based on this theory, we predict a surprising effect: carrier doping, which is commonly believed to suppress electric polarization, can lead to enhanced polarization in CuInP2S6. Our first-principles simulations confirm this unusual effect and further show that an elevated hole doping level can cause electric polarization to give way to emerging ferromagnetism. Our results not only pave a way to realize ferroelectric metals, but also broaden the scope of magnetoelectric coupling mechanisms and may help enrich the potential applications of layered ferroelectric materials in the future.

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