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    Fully compensated ferrimagnetism via local orbital-driven clusters

    Yurong Ruan1,*, Zilong Liao1,*, Tao Feng1,†, Ke Zhong1, Bing Wen1, Weishu Liu1,‡, and Wenqing Zhang1,2,§

    • *These authors contributed equally to this work.
    • †Contact author: fengt@sustech.edu.cn
    • ‡Contact author: liuws@sustech.edu.cn
    • §Contact author: zhangwq@sustech.edu.cn

    Phys. Rev. B 114, 094432 – Published 25 August, 2026

    DOI: https://doi.org/10.1103/wsls-cpg2

    Abstract

    In fully compensated ferrimagnets (FCFs), the coexistence of vanishing net magnetization and spin polarization provides a unique platform for spintronics. However, their realization remains hindered by the stringent sublattice constraints and electron-counting requirements. Here, we propose a design strategy for FCFs in disordered, off-stoichiometry Heusler-like compounds, using TiCoxCuySn (1<x+y<2) as a prototype. We show that the vanishing magnetization is rooted in local orbital-driven exchange between partially occupied Co-3d e orbitals (dx2−y2,dz2) in inequivalent Co environments, while Cu+ provides the charge-compensation degree of freedom. This mechanism manifests as short-range, self-compensated magnetic clusters associated with off-stoichiometric Co/Cu/vacancy configurations within an ordered cubic framework, enabling a zero-net-moment state across a broad, continuously tunable compositional window. Experimental measurements support a compensated ferrimagnetic state with vanishing macroscopic magnetization, together with a low-temperature logarithmic magnetic-scattering contribution that is progressively suppressed by magnetic field. Our findings demonstrate that local orbital-driven clusters enable fully compensated ferrimagnetism beyond the rigid integer-valence-electron-count Slater-Pauling constraint, providing a powerful pathway for engineering functional FCFs.

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