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

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.