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Magnetic materials combining spin-glass behavior with hard-magnet coercivity are important for fundamental and applied research. Herein, we report spin glass behaviors coupled to remarkably large intrinsic coercivity values of 302.4 kA/m (Hc = 3.80 kOe) in Mo1.5Mn1.5B2 and 175.1 kA/m (Hc = 2.20 kOe) in W1.5Mn1.5B2. Both phases belong to the Mo2FeB2-type structure known for enabling excellent structural properties and predicted altermagnetic candidates. Single-phase products were obtained via a compositionally tuned solid-state route that resolves prior phase-purity challenges. Temperature-dependent susceptibility measurements revealed spin-glass behavior below the freezing temperatures Tg = 29 K for Mo1.5Mn1.5B2 and Tg = 43 K (reentrant cluster spin glass) as well as a ferromagnetic (FM) transition at 70 K for W1.5Mn1.5B2. AC susceptibility measurements exhibited frequency-dependent peaks that shifted to higher temperatures with increasing frequency, confirming the presence of dynamic spin freezing in both compounds. DFT calculations confirmed the presence of strongly competing FM and antiferromagnetic (AFM) interactions leading to competing AFM/FM/FiM orderings with a greater spin-exchange energy (ΔEₑₓ = 28-98 meV/f.u.) for FiM/AFM compared to FM in Mo1.5Mn1.5B2 and even greater ΔEₑₓ = 53-131 meV/f.u. in W1.5Mn1.5B2. The magnetocrystalline anisotropy energy (MAE) is uniaxial, favoring the c-axis, with MAE = -0.17 meV/f.u. (Mo) and -0.10 meV/f.u. (W), which align well with the large hysteresis found experimentally, while the unexpectedly larger coercivity of Mo1.5Mn1.5B2 correlates with its greater Eₑₓ. These findings enable the development of Mo2FeB2-type multifunctional materials, expanding their applications beyond traditional structural material properties.

権利情報:

• In Copyright
  

  This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © 2025 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/jacs.5c12552.

キーワード: spin glasses, anisotropic magnets, magnetic properties, Mo2FeB2 type

刊行年月日: 2025-11-05

出版者: American Chemical Society (ACS)

掲載誌:

• Journal of the American Chemical Society (ISSN: 00027863) vol. 147 issue. 44 p. 40562-40575

研究助成金:

• JST-Mirai Program JPMJMI19A1
• Committee on Research
• San Diego Supercomputer Center

原稿種別: 著者最終稿 (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.5868

公開URL: https://doi.org/10.1021/jacs.5c12552

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更新時刻: 2026-04-30 12:01:11 +0900

MDRでの公開時刻: 2026-10-27 08:28:10 +0900