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; Yi Zheng

doi:10.1038/s41467-024-47373-7

Article 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 (National Institute for Materials Science) ; Takashi Taniguchi (National Institute for Materials Science) ; Yunhao Lu ; Chuanhong Jin ; Dawei Wang ; Yi Zheng

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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, Yi Zheng. Ferrielectricity controlled widely-tunable magnetoelectric coupling in van der Waals multiferroics. Nature Communications. 2024, 15 (1), 3029. https://doi.org/10.1038/s41467-024-47373-7

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The discovery of various primary ferroic phases in atomically-thin van der Waals (vdW) crystals have created a new two-dimensional (2D) wonderland for exploring and manipulating exotic quantum phases. It may also bring technical breakthroughs in device applications, as evident by prototype functionalities of giant tunnelling magnetoresistance, gate-tunable ferromagnetism and non-volatile ferroelectric memory etc. However, 2D multiferroics with effective magnetoelectric coupling (MEC), which ultimately decides the future of multiferroic-based information technology, has not been realized yet. Here, we show that an unconventional MEC mechanism interlocked with heterogeneous ferrielectric (FiE) transitions emerges at the 2D limit in vdW monolayers of CuCrP2S6 with inherent ferromagnetism and antiferroelectricity. Distinct from the homogeneous antiferroelectric (AFE) bulk, thin-layer CuCrP2S6 under external electric field makes layer-dependent heterogeneous FiE transitions, minimizing the depolarization effect introduced by the rearrangements of Cu+ ions within the ferromagnetic vdW cages of CrS6 and P2S6 octahedrons. The resulting FiE phases are characterized by substantially reduced interlayer magnetic coupling energy of nearly 50% with a moderate electric field of 0.3 V/nm, producing widely-tunable MEC which can be further engineered by asymmetrical electrode work functions.

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