Surprising pressure-induced magnetic transformations from helimagnetic order to antiferromagnetic state in NiI2

Qiye Liu, Wenjie Su, Yue Gu, Xi Zhang, Xiuquan Xia, Le Wang, Ke Xiao, Naipeng Zhang, Xiaodong Cui, Mingyuan Huang, Chengrong Wei, Xiaolong Zou (), Bin Xi (), Jia-Wei Mei () and Jun-Feng Dai ()
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Qiye Liu: Shenzhen Technology University
Wenjie Su: Southern University of Science and Technology
Yue Gu: Tsinghua University
Xi Zhang: Southern University of Science and Technology
Xiuquan Xia: Southern University of Science and Technology
Le Wang: Southern University of Science and Technology
Ke Xiao: Max Planck Institute of Microstructure Physics
Naipeng Zhang: Southern University of Science and Technology
Xiaodong Cui: Pokfulam Road
Mingyuan Huang: Southern University of Science and Technology
Chengrong Wei: Shenzhen Technology University
Xiaolong Zou: Tsinghua University
Bin Xi: Yangzhou University
Jia-Wei Mei: Southern University of Science and Technology
Jun-Feng Dai: Shenzhen Technology University

Nature Communications, 2025, vol. 16, issue 1, 1-8

Abstract: Abstract Interlayer magnetic interactions play a pivotal role in determining the magnetic arrangement within van der Waals (vdW) magnets, and the remarkable tunability of these interactions through applied pressure further enhances their significance. Here, we investigate NiI2 flakes, a representative vdW magnet, under hydrostatic pressures up to 11 GPa. We reveal a notable increase in magnetic transition temperatures for both helimagnetic and antiferromagnetic states, and find that a reversible transition between helimagnetic and antiferromagnetic (AFM) phases at approximately 7 GPa challenges established theoretical and experimental expectations. While the increase in transition temperature aligns with pressure-enhanced overall exchange interaction strengths, we identify the significant role of the second-nearest neighbor interlayer interaction $${J}_{2}^{\perp }$$ J 2 ⊥ , which competes with intra-layer frustration and favors the AFM state as demonstrated in the Monte Carlo simulations. Experimental and simulated results converge on the existence of an intermediate helimagnetic ordered state in NiI2 before transitioning to the AFM state. These findings underscore the pivotal role of interlayer interactions in shaping the magnetic ground state, providing fresh perspectives for innovative applications in nanoscale magnetic device design.

Date: 2025
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DOI: 10.1038/s41467-025-59561-0

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