Fully compensated ferrimagnetism via local orbital-driven clusters
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 () as a prototype. We show that the vanishing magnetization is rooted in local orbital-driven exchange between partially occupied Co- orbitals () in inequivalent Co environments, while 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.