Ferrielectricity controlled widely-tunable magnetoelectric coupling in van der Waals multiferroics

Qifeng Hu, Yuqiang Huang, Yang Wang, Sujuan Ding, Minjie Zhang, Chenqiang Hua, Linjun Li (), Xiangfan Xu, Jinbo Yang, Shengjun Yuan, Kenji Watanabe, Takashi Taniguchi, Yunhao Lu (), Chuanhong Jin (), Dawei Wang and Yi Zheng ()
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Qifeng Hu: Zhejiang University
Yuqiang Huang: Zhejiang University
Yang Wang: Zhejiang University
Sujuan Ding: Zhejiang University
Minjie Zhang: Zhejiang University
Chenqiang Hua: Zhejiang University
Linjun Li: Zhejiang University
Xiangfan Xu: Tongji University
Jinbo Yang: Peking University
Shengjun Yuan: Wuhan University
Kenji Watanabe: National Institute for Materials Science
Takashi Taniguchi: National Institute for Materials Science
Yunhao Lu: Zhejiang University
Chuanhong Jin: Zhejiang University
Dawei Wang: Zhejiang University
Yi Zheng: Zhejiang University

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract The discovery of various primary ferroic phases in atomically-thin van der Waals crystals have created a new two-dimensional wonderland for exploring and manipulating exotic quantum phases. It may also bring technical breakthroughs in device applications, as evident by prototypical functionalities of giant tunneling magnetoresistance, gate-tunable ferromagnetism and non-volatile ferroelectric memory etc. However, two-dimensional multiferroics with effective magnetoelectric coupling, which ultimately decides the future of multiferroic-based information technology, has not been realized yet. Here, we show that an unconventional magnetoelectric coupling mechanism interlocked with heterogeneous ferrielectric transitions emerges at the two-dimensional limit in van der Waals multiferroic CuCrP2S6 with inherent antiferromagnetism and antiferroelectricity. Distinct from the homogeneous antiferroelectric bulk, thin-layer CuCrP2S6 under external electric field makes layer-dependent heterogeneous ferrielectric transitions, minimizing the depolarization effect introduced by the rearrangements of Cu+ ions within the ferromagnetic van der Waals cages of CrS6 and P2S6 octahedrons. The resulting ferrielectric phases are characterized by substantially reduced interlayer magnetic coupling energy of nearly 50% with a moderate electric field of 0.3 V nm−1, producing widely-tunable magnetoelectric coupling which can be further engineered by asymmetrical electrode work functions.

Date: 2024
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DOI: 10.1038/s41467-024-47373-7

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