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We have successfully synthesized four Mo$_3$O$_8$-type cluster Mottinsulators (CMI) by intercalating lithium into nonmagnetic precursors toregulate the Mo$_3$ cluster valence. The resulting materials areLi$_{1+x}$$R$Mo$_3$O$_8$ ($R$ = Sc, Y, Lu) and Li$_x$Zn$_2$Mo$_3$O$_8$. Ourmagnetic susceptibility measurements revealed that these materials displaycharacteristics akin to a valence bond glass state and suggest the presence ofshort-range ordering when the Mo$_3$ cluster valence approximates its idealvalue. These findings challenge the prevailing belief that the plaquette chargeordering state is an inherent feature of Mo$_3$O$_8$-type CMI. Instead, theyunderscore the importance of Mo$_3$ cluster valence in determining the physicalproperties of these systems. These insights furnish a fresh understanding ofthe Mo$_3$O$_8$-type CMI and open new research opportunities in highlyfrustrated magnetism.

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