Spin Frustration and Unconventional Surface Spin Canting State in Van der Waals Ferromagnet/Antiferromagnet Heterostructures

Journal Article · Wed Oct 01 00:00:00 EDT 2025 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202504700· OSTI ID:2587741

Wang, Tianye; Li, Qian; Yang, Mengmeng; Sun, Yu; N'Diaye, Alpha T; Klewe, Christoph; Scholl, Andreas; Chen, Xianzhe; Huang, Xiaoxi; Zhang, Hongrui; Yang, Santai; Lee, Ji‐Eun; Balakrishnan, Dhanvanth; Zhang, Xixiang; Hwang, Chanyong; Shafer, Padraic C; Crommie, Michael F; Ramesh, Ramamoorthy; Qiu, Zi Q

Atomically flat surfaces of van der Waals (vdW) materials pave an avenue for addressing a long-standing fundamental issue of how a compensated antiferromagnet (AFM) surface frustrates a ferromagnetic (FM) overlayer in FM/AFM heterostructures. We investigate Fe5GeTe2/NiPS3 vdW heterostructures by characterizing AFM and FM spins separately. We find that in-plane zig-zag AFM NiPS3 develops three equivalent AFM domains, which are robust against external magnetic field and magnetic coupling with Fe5GeTe2. Moreover, evidence is provided of in-plane-AFM-induced perpendicular magnetic anisotropy (PMA) in adjacent Fe5GeTe2, and an unconventional out-of-plane surface spin canting state with the Fe5GeTe2 spins spatially turn from out-of-plane direction near the interface to in-plane direction away from the interface in Fe5GeTe2/NiPS3. The out-of-plane surface spin canting is a unique property of spin frustration in vdW magnetic heterostructures.

• Research Organization: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
• Sponsoring Organization: US Department of Energy; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Materials Sciences & Engineering Division (SC-22.2)
• Grant/Contract Number: AC02-05CH11231
• OSTI ID: 2587741
• Journal Information: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 42 Vol. 37
• Country of Publication: United States
• Language: English