Long-range magnetoelectricity in type-II multiferroic NiI <sub>2</sub>

W Weiyi Pan (Department of Physics, State Key Laboratory of Low Dimensional Quantum Physics, Tsinghua University) Z Zefeng Chen (Department of Physics, Key Laboratory of Computational Physical Sciences (Ministry of Education), Institute of Computational Physical Sciences, State Key Laboratory of Surface Physics, Fudan University) T Tianxing Jiang (Department of Physics, Key Laboratory of Computational Physical Sciences (Ministry of Education), Institute of Computational Physical Sciences, State Key Laboratory of Surface Physics, Fudan University) H Haitao Wang (Department of Central Laboratory, College & Hospital of Stomatology, Anhui Provincial Key Laboratory of Oral Diseases Research, Anhui Medical University) D Dezhao Wu (Department of Physics, State Key Laboratory of Low Dimensional Quantum Physics, Tsinghua University) W Weiqin Zhu (Department of Physics, Key Laboratory of Computational Physical Sciences (Ministry of Education), Institute of Computational Physical Sciences, State Key Laboratory of Surface Physics, Fudan University) Z Zhiming Xu (Department of Neurosurgery, Shanghai Sixth People’s Hospital Affiliated to Shanghai Jiao Tong University School of Medicine) L Lianchuang Li (Department of Physics, Key Laboratory of Computational Physical Sciences (Ministry of Education), Institute of Computational Physical Sciences, State Key Laboratory of Surface Physics, Fudan University) J Junsheng Feng (School of Physics and Materials Engineering, Hefei Normal University) T Tong Zhang B Bing-Lin Gu (Department of Physics, State Key Laboratory of Low Dimensional Quantum Physics, Tsinghua University) W Wenhui Duan (State Key Laboratory of Low Dimensional Quantum Physics and Department of Physics) C Changsong Xu (Department of Physics, Key Laboratory of Computational Physical Sciences (Ministry of Education), Institute of Computational Physical Sciences, State Key Laboratory of Surface Physics, Fudan University)

Abstract

Type-II multiferroics, where spin order induces ferroelectricity, exhibit strong magnetoelectric coupling. However, for the typical 2D type-II multiferroic NiI 2 , the underlying magnetoelectric mechanism remains unclear. Here, applying generalized spin-current model, together with first-principles calculations and a tight-binding approach, we build a comprehensive magnetoelectric model for spin-induced polarization. Such model reveals that third-nearest-neighbor spin pairs provide an unexpectedly strong contribution to the electric polarization, which rivals that of the first-nearest neighbors. Adopting such model, both experimental-detectable bound charge induced by spin-induced polarization at the spiral domain boundary, as well as polar vortex lattice induced by magnetic skyrmion lattice under moderate magnetic field, are predicted. Furthermore, by analyzing the orbital-resolved contributions to polarization, our tight-binding model reveals that the long-range magnetoelectric coupling is enabled by the strong e g - p hopping of NiI 2 . These findings can guide the identification and design of strongly magnetoelectric multiferroics.

Article Details

Volume / Issue Vol. 123, Issue 30
Published July 28, 2026
ISSN 0027-8424
Publisher National Academy of Sciences

Authors (13)

W

Weiyi Pan

Department of Physics, State Key Laboratory of Low Dimensional Quantum Physics, Tsinghua University

Z

Zefeng Chen

Department of Physics, Key Laboratory of Computational Physical Sciences (Ministry of Education), Institute of Computational Physical Sciences, State Key Laboratory of Surface Physics, Fudan University

T

Tianxing Jiang

Department of Physics, Key Laboratory of Computational Physical Sciences (Ministry of Education), Institute of Computational Physical Sciences, State Key Laboratory of Surface Physics, Fudan University

H

Haitao Wang

Department of Central Laboratory, College & Hospital of Stomatology, Anhui Provincial Key Laboratory of Oral Diseases Research, Anhui Medical University

D

Dezhao Wu

Department of Physics, State Key Laboratory of Low Dimensional Quantum Physics, Tsinghua University

W

Weiqin Zhu

Department of Physics, Key Laboratory of Computational Physical Sciences (Ministry of Education), Institute of Computational Physical Sciences, State Key Laboratory of Surface Physics, Fudan University

Z

Zhiming Xu

Department of Neurosurgery, Shanghai Sixth People’s Hospital Affiliated to Shanghai Jiao Tong University School of Medicine

L

Lianchuang Li

Department of Physics, Key Laboratory of Computational Physical Sciences (Ministry of Education), Institute of Computational Physical Sciences, State Key Laboratory of Surface Physics, Fudan University

J

Junsheng Feng

School of Physics and Materials Engineering, Hefei Normal University

T

Tong Zhang

B

Bing-Lin Gu

Department of Physics, State Key Laboratory of Low Dimensional Quantum Physics, Tsinghua University

W

Wenhui Duan

State Key Laboratory of Low Dimensional Quantum Physics and Department of Physics

C

Changsong Xu

Department of Physics, Key Laboratory of Computational Physical Sciences (Ministry of Education), Institute of Computational Physical Sciences, State Key Laboratory of Surface Physics, Fudan University