Observation of stacking engineered magnetic phase transitions within moiré supercells of twisted van der Waals magnets

Senlei Li, Zeliang Sun, Nathan J. McLaughlin, Afsana Sharmin, Nishkarsh Agarwal, Mengqi Huang, Suk Hyun Sung, Hanyi Lu, Shaohua Yan, Hechang Lei, Robert Hovden, Hailong Wang, Hua Chen, Liuyan Zhao () and Chunhui Rita Du ()
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Senlei Li: Georgia Institute of Technology
Zeliang Sun: the University of Michigan
Nathan J. McLaughlin: University of California, San Diego, La Jolla
Afsana Sharmin: Colorado State University
Nishkarsh Agarwal: University of Michigan
Mengqi Huang: Georgia Institute of Technology
Suk Hyun Sung: University of Michigan
Hanyi Lu: University of California, San Diego, La Jolla
Shaohua Yan: Renmin University of China
Hechang Lei: Renmin University of China
Robert Hovden: University of Michigan
Hailong Wang: Georgia Institute of Technology
Hua Chen: Colorado State University
Liuyan Zhao: the University of Michigan
Chunhui Rita Du: Georgia Institute of Technology

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

Abstract: Abstract Recent demonstrations of moiré magnetism, featuring exotic phases with noncollinear spin order in the twisted van der Waals (vdW) magnet chromium triiodide CrI3, have highlighted the potential of twist engineering of magnetic (vdW) materials. However, the local magnetic interactions, spin dynamics, and magnetic phase transitions within and across individual moiré supercells remain elusive. Taking advantage of a scanning single-spin magnetometry platform, here we report observation of two distinct magnetic phase transitions with separate critical temperatures within a moiré supercell of small-angle twisted double trilayer CrI3. By measuring temperature-dependent spin fluctuations at the coexisting ferromagnetic and antiferromagnetic regions in twisted CrI3, we explicitly show that the Curie temperature of the ferromagnetic state is higher than the Néel temperature of the antiferromagnetic one by ~10 K. Our mean-field calculations attribute such a spatial and thermodynamic phase separation to the stacking order modulated interlayer exchange coupling at the twisted interface of moiré superlattices.

Date: 2024
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DOI: 10.1038/s41467-024-49942-2

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