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    Negative magnetization, magnetization switching, and associated exchange interactions in the Mn self-doped double perovskites Gd2Ni2−xMnxO6 (1.0≤x≤1.6)

    Canglong Li1,*, Wenqian Yang1, Xuechi Lu1, Boyuan Zou1, Xinshuai Niu1, Jie Chen1, Bing Zhang1, Kexin Wen1, and Godfrey Okumu Barasa2

    • *Contact author: licanglong@xynu.edu.cn

    Phys. Rev. B 113, 014411 – Published 9 January, 2026

    DOI: https://doi.org/10.1103/w4sl-l8y4

    Abstract

    Heavy rare-earth-based quaternary double perovskite with the formula R2BB′O6 has attracted great attention due to its multiple magnetic exchange interactions, intriguing type of magnetic ordering, and antisite disorder. In this work, magnetic behaviors, magnetic-field-assisted switching effect, and associated exchange interactions in Mn self-doped double perovskites Gd2Ni2−xMnxO6 (1.0≤x≤1.6) are investigated by using different protocols of DC and AC magnetic measurements. Experiments indicate that negative magnetization effects characterized by MFC<0 under moderate positive magnetic fields are observed from x=1.3 up to x=1.5. The repeatability of M(T) under different magnetic fields and its mirror symmetry about the temperature axis under ±Hcool signify the intrinsic nature of the effect. The manipulability of magnetization polarity is demonstrated by the magnetic-field-assisted switching effect, indicating promising application prospects in spintronics devices. The simultaneous decrease of both MFC and transition temperature TC by Mn self-doping suggests the weakening of Ni2+−Mn4+ ferromagnetic interaction due to the increase in antisite disorder, which is considered as a triggering factor of the negative magnetization. Therefore, the observed effect is regarded as arising from the negative exchange coupling between Gd3+ and Ni2+/Mn4+ local sublattice moments, which have different temperature dependence according to the Néel molecular field theory.

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