Spin fluctuations steer the electronic behavior in the FeSb 3 skutterudite

Skutterudites are promising materials for thermoelectric and spintronics applications. Here, we explore spin fluctuations in the FeSb 3 skutterudite and their effect on its electronic structure using Hubbard-corrected density-functional theory calculations. We identify multiple magnetic- and charge-disproportionated configurations, with an antiferromagnetic metallic ground state. Paramagnetic fluctuations modeled through a special quasirandom spin structure open a 61 meV gap, consistent with experiments. This state features nondegenerate spin channels and band-avoided crossings, resembling a Luttinger-compensated ferrimagnet. Mapping the electronic structure to a Heisenberg Hamiltonian fails to explain the low Néel temperature ( ≲ 10 K ), suggesting that factors such as stoichiometry and magnetic exchange frustration may play an important role, calling for more detailed experimental investigations.