Impact of Oxidation State on the Valence-bond-glass Physics in the lithium-intercalated Mo$_3$O$_8$ Cluster Mott Insulators

Abstract: We have successfully synthesized four Mo$3$O$_8$-type cluster Mott insulators (CMI) by intercalating lithium into nonmagnetic precursors to regulate the Mo$_3$ cluster valence. The resulting materials are Li${1+x}$$R$Mo$_3$O$_8$ ($R$ = Sc, Y, Lu) and Li$_x$Zn$_2$Mo$_3$O$_8$. Our magnetic susceptibility measurements revealed that these materials display characteristics akin to a valence bond glass state and suggest the presence of short-range ordering when the Mo$_3$ cluster valence approximates its ideal value. These findings challenge the prevailing belief that the plaquette charge ordering state is an inherent feature of Mo$_3$O$_8$-type CMI. Instead, they underscore the importance of Mo$_3$ cluster valence in determining the physical properties of these systems. These insights furnish a fresh understanding of the Mo$_3$O$_8$-type CMI and open new research opportunities in highly frustrated magnetism.