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

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

doi:10.1002/adma.202504700

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

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

Department of Physics

University of California at Berkeley
Lawrence Berkeley National Laboratory
University of Science and Technology of China
Anhui University
ShanghaiTech University
CAS - Ningbo Institute of Material Technology and Engineering
King Abdullah University of Science and Technology
Korea Research Institute of Standards and Science

Research output: Contribution to journal › Article › peer-review

2 Scopus citations

Abstract

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.

Original language	English
Article number	e04700
Journal	Advanced Materials
Volume	37
Issue number	42
DOIs	https://doi.org/10.1002/adma.202504700
State	Published - 23 Oct 2025

Keywords

spin frustration
spin texture
synchrotron radiation
van der Waals magnetic heterostructures

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10.1002/adma.202504700

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Wang, T., Li, Q., Yang, M., Sun, Y., N'Diaye, A. T., Klewe, C., Scholl, A., Chen, X., Huang, X., Zhang, H., Yang, S., Lee, J. E., Balakrishnan, D., Zhang, X., Hwang, C., Shafer, P. C., Crommie, M. F., Ramesh, R., & Qiu, Z. Q. (2025). Spin Frustration and Unconventional Surface Spin Canting State in Van der Waals Ferromagnet/Antiferromagnet Heterostructures. Advanced Materials, 37(42), Article e04700. https://doi.org/10.1002/adma.202504700

@article{df0461c96a1a46ab8b7d16d2448b2fcd,

title = "Spin Frustration and Unconventional Surface Spin Canting State in Van der Waals Ferromagnet/Antiferromagnet Heterostructures",

abstract = "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.",

keywords = "spin frustration, spin texture, synchrotron radiation, van der Waals magnetic heterostructures",

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

note = "Publisher Copyright: {\textcopyright} 2025 Wiley-VCH GmbH.",

year = "2025",

month = oct,

day = "23",

doi = "10.1002/adma.202504700",

language = "English",

volume = "37",

journal = "Advanced Materials",

issn = "0935-9648",

publisher = "Wiley-Blackwell",

number = "42",

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Wang, T, Li, Q, Yang, M, Sun, Y, N'Diaye, AT, Klewe, C, Scholl, A, Chen, X, Huang, X, Zhang, H, Yang, S, Lee, JE, Balakrishnan, D, Zhang, X, Hwang, C, Shafer, PC, Crommie, MF, Ramesh, R & Qiu, ZQ 2025, 'Spin Frustration and Unconventional Surface Spin Canting State in Van der Waals Ferromagnet/Antiferromagnet Heterostructures', Advanced Materials, vol. 37, no. 42, e04700. https://doi.org/10.1002/adma.202504700

TY - JOUR

T1 - Spin Frustration and Unconventional Surface Spin Canting State in Van der Waals Ferromagnet/Antiferromagnet Heterostructures

AU - Wang, Tianye

AU - Li, Qian

AU - Yang, Mengmeng

AU - Sun, Yu

AU - N'Diaye, Alpha T.

AU - Klewe, Christoph

AU - Scholl, Andreas

AU - Chen, Xianzhe

AU - Huang, Xiaoxi

AU - Zhang, Hongrui

AU - Yang, Santai

AU - Lee, Ji Eun

AU - Balakrishnan, Dhanvanth

AU - Zhang, Xixiang

AU - Hwang, Chanyong

AU - Shafer, Padraic C.

AU - Crommie, Michael F.

AU - Ramesh, Ramamoorthy

AU - Qiu, Zi Q.

PY - 2025/10/23

Y1 - 2025/10/23

N2 - 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.

AB - 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.

KW - spin frustration

KW - spin texture

KW - synchrotron radiation

KW - van der Waals magnetic heterostructures

UR - https://www.scopus.com/pages/publications/105012305082

U2 - 10.1002/adma.202504700

DO - 10.1002/adma.202504700

M3 - Article

C2 - 40746208

AN - SCOPUS:105012305082

SN - 0935-9648

VL - 37

JO - Advanced Materials

JF - Advanced Materials

IS - 42

M1 - e04700

ER -

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

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Keywords

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