Sequential Charge Transfer and Magnetic Ordering in Quasi-One-Dimensional Antiferromagnet CrSbS3

Abstract

Charge transfer and magnetic ordering are two profound condensed matter phenomena that impart distinct structures and properties to materials. However, such two effects rarely occur successively within a single material. Here, we present a unique case of temperature-induced sequential charge transfer and magnetic ordering in antiferromagnetic CrSbS₃ with quasi-one-dimensional structure. Intriguingly, the contrasting effects of charge transfer between Cr and [Sb₂S₆] units and antiferromagnetic transition on lattice expansion result in diverse thermal expansion behaviors of lattice parameters, which ultimately leads to an anti-Invar effect on the lattice volume. Neutron powder diffraction further unravels a C-type antiferromagnetic order. Moreover, pressure regulation can also induce similar volume collapse, implying potential valence and spin-state transitions. The multiple electronic transitions observed in CrSbS₃ offer a valuable platform for deciphering the interweaving among charge, spin, and lattice degrees of freedom, and shed a new light for exploring novel quantum phenomena in more low-dimensional van der Waals materials.