Bilayer Kagome Ferrimagnet Exhibiting Exceptional Spontaneous Exchange Bias in TbMn6(Ge,Ga)6

Hankun Xu; Wenjie Li; Junjie Chen; Sergii Khmelevskyi; Dmitry Khalyavin; Pascal Manuel; Chuanying Xi; Shogo Kawaguchi; Jing Chen; Wanda Yang; Qinghua Zhang; Yili Cao; Chengyi Yu; Yang Ren; Kun Lin; Xianran Xing

doi:10.1021/jacs.4c17505

Bilayer Kagome Ferrimagnet Exhibiting Exceptional Spontaneous Exchange Bias in TbMn₆(Ge,Ga)₆

Hankun Xu (Co-first Author)
, Wenjie Li (Co-first Author)
, Junjie Chen
, Sergii Khmelevskyi
, Dmitry Khalyavin
, Pascal Manuel
, Chuanying Xi
, Shogo Kawaguchi
, Jing Chen
, Wanda Yang
, Qinghua Zhang
, Yili Cao
, Chengyi Yu
, Yang Ren
, Kun Lin^*
, Xianran Xing^*

^*Corresponding author for this work

Department of Physics

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

6 Citations (Scopus)

Abstract

Manipulating interlayer interactions in two-dimensional (2D) materials has led to intriguing behaviors. Borrowing these 2D signatures to bulk materials is likely to unlock exceptional properties. Here, we report an emergent 2D-like bilayer Kagome ferrimagnet through reducing the interbilayer magnetic interaction to nearly zero. This concept is realized within bulk TbMn₆(Ge,Ga)₆ compounds, characterized by an isolated and pure Mn Kagome lattice, simply by the chemical substitution of Ge with Ga. Specifically, the targeted compound TbMn₆Ge₅Ga₁ exhibits a giant spontaneous exchange bias (SEB) of approximately 1.6 T, which is more than twice that observed in known materials. Field-dependent neutron diffraction reveals the robust nature of the compensated ferrimagnetic (FiM), characterized by almost two-thirds of the moments being pinned and irreversible under fields up to 9 T. Through magnetic and structural analysis, alongside theoretical calculations, we demonstrate that the substantial SEB is related to the intense competition between local robust and weak FiM states within the bilayer Kagome configuration, which are stabilized by an incommensurate spin arrangement. The concept of a bilayer Kagome magnet offers new opportunities for discovering attractive properties in 2D-like materials. © 2025 American Chemical Society.

Original language	English
Pages (from-to)	11941-11948
Journal	Journal of the American Chemical Society
Volume	147
Issue number	14
Online published	27 Mar 2025
DOIs	https://doi.org/10.1021/jacs.4c17505
Publication status	Published - 9 Apr 2025

Funding

This research was supported by the National Key R&D Program of China (2020YFA0406202), the National Natural Science Foundation of China (22371014, 22090042, and 21971009), Guangxi BaGui Scholars Special Funding (2019M660446), and the Fundamental Research Funds for the Central Universities, China (GJRC2023003, FRF-EYIT-23-03). The temperature dependence of neutron diffraction and in situ neutron diffraction applied field experiments were carried out at the WISH of ISIS (Proposal No. 22000036). The synchrotron radiation diffraction experiments were performed at the BL02B2 and BL44B2 of SPring-8 with the approval of the Japan Synchrotron Radiation Research Institute (JASRI) (Proposal No. 2023B1810 and No. 2024A1556, respectively). The authors acknowledge Dr. Langsheng Ling for performing the steady high-field measurement equipped with the water-cooled magnet WM5 at the High Magnetic Field Laboratory, Chinese Academy of Sciences in Hefei, China. The authors acknowledge Prof. Junfeng Wang, Dr. Chao Dong, and graduate student Yanfa Feng for assisting in collecting the pulsed high magnetic field data, which was generated by the nondestructive short-pulse magnet at the Wuhan National High Magnetic Field Center (WHMFC), China. The authors also acknowledge Prof. Congling Yin (Guilin University of Technology), Prof. Sihao Deng, and Prof. Qingzhen Huang (China Spallation Neutron Source) for their guidance in the neutron diffraction refinement.

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Xu, H., Li, W., Chen, J., Khmelevskyi, S., Khalyavin, D., Manuel, P., Xi, C., Kawaguchi, S., Chen, J., Yang, W., Zhang, Q., Cao, Y., Yu, C., Ren, Y., Lin, K., & Xing, X. (2025). Bilayer Kagome Ferrimagnet Exhibiting Exceptional Spontaneous Exchange Bias in TbMn₆(Ge,Ga)₆. Journal of the American Chemical Society, 147(14), 11941-11948. https://doi.org/10.1021/jacs.4c17505

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abstract = "Manipulating interlayer interactions in two-dimensional (2D) materials has led to intriguing behaviors. Borrowing these 2D signatures to bulk materials is likely to unlock exceptional properties. Here, we report an emergent 2D-like bilayer Kagome ferrimagnet through reducing the interbilayer magnetic interaction to nearly zero. This concept is realized within bulk TbMn6(Ge,Ga)6 compounds, characterized by an isolated and pure Mn Kagome lattice, simply by the chemical substitution of Ge with Ga. Specifically, the targeted compound TbMn6Ge5Ga1 exhibits a giant spontaneous exchange bias (SEB) of approximately 1.6 T, which is more than twice that observed in known materials. Field-dependent neutron diffraction reveals the robust nature of the compensated ferrimagnetic (FiM), characterized by almost two-thirds of the moments being pinned and irreversible under fields up to 9 T. Through magnetic and structural analysis, alongside theoretical calculations, we demonstrate that the substantial SEB is related to the intense competition between local robust and weak FiM states within the bilayer Kagome configuration, which are stabilized by an incommensurate spin arrangement. The concept of a bilayer Kagome magnet offers new opportunities for discovering attractive properties in 2D-like materials. {\textcopyright} 2025 American Chemical Society.",

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Bilayer Kagome Ferrimagnet Exhibiting Exceptional Spontaneous Exchange Bias in TbMn₆(Ge,Ga)₆. / Xu, Hankun (Co-first Author); Li, Wenjie (Co-first Author); Chen, Junjie et al.
In: Journal of the American Chemical Society, Vol. 147, No. 14, 09.04.2025, p. 11941-11948.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Bilayer Kagome Ferrimagnet Exhibiting Exceptional Spontaneous Exchange Bias in TbMn6(Ge,Ga)6

AU - Xu, Hankun

AU - Li, Wenjie

AU - Chen, Junjie

AU - Khmelevskyi, Sergii

AU - Khalyavin, Dmitry

AU - Manuel, Pascal

AU - Xi, Chuanying

AU - Kawaguchi, Shogo

AU - Chen, Jing

AU - Yang, Wanda

AU - Zhang, Qinghua

AU - Cao, Yili

AU - Yu, Chengyi

AU - Ren, Yang

AU - Lin, Kun

AU - Xing, Xianran

PY - 2025/4/9

Y1 - 2025/4/9

N2 - Manipulating interlayer interactions in two-dimensional (2D) materials has led to intriguing behaviors. Borrowing these 2D signatures to bulk materials is likely to unlock exceptional properties. Here, we report an emergent 2D-like bilayer Kagome ferrimagnet through reducing the interbilayer magnetic interaction to nearly zero. This concept is realized within bulk TbMn6(Ge,Ga)6 compounds, characterized by an isolated and pure Mn Kagome lattice, simply by the chemical substitution of Ge with Ga. Specifically, the targeted compound TbMn6Ge5Ga1 exhibits a giant spontaneous exchange bias (SEB) of approximately 1.6 T, which is more than twice that observed in known materials. Field-dependent neutron diffraction reveals the robust nature of the compensated ferrimagnetic (FiM), characterized by almost two-thirds of the moments being pinned and irreversible under fields up to 9 T. Through magnetic and structural analysis, alongside theoretical calculations, we demonstrate that the substantial SEB is related to the intense competition between local robust and weak FiM states within the bilayer Kagome configuration, which are stabilized by an incommensurate spin arrangement. The concept of a bilayer Kagome magnet offers new opportunities for discovering attractive properties in 2D-like materials. © 2025 American Chemical Society.

AB - Manipulating interlayer interactions in two-dimensional (2D) materials has led to intriguing behaviors. Borrowing these 2D signatures to bulk materials is likely to unlock exceptional properties. Here, we report an emergent 2D-like bilayer Kagome ferrimagnet through reducing the interbilayer magnetic interaction to nearly zero. This concept is realized within bulk TbMn6(Ge,Ga)6 compounds, characterized by an isolated and pure Mn Kagome lattice, simply by the chemical substitution of Ge with Ga. Specifically, the targeted compound TbMn6Ge5Ga1 exhibits a giant spontaneous exchange bias (SEB) of approximately 1.6 T, which is more than twice that observed in known materials. Field-dependent neutron diffraction reveals the robust nature of the compensated ferrimagnetic (FiM), characterized by almost two-thirds of the moments being pinned and irreversible under fields up to 9 T. Through magnetic and structural analysis, alongside theoretical calculations, we demonstrate that the substantial SEB is related to the intense competition between local robust and weak FiM states within the bilayer Kagome configuration, which are stabilized by an incommensurate spin arrangement. The concept of a bilayer Kagome magnet offers new opportunities for discovering attractive properties in 2D-like materials. © 2025 American Chemical Society.

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