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LiZn$_2$Mo$_3$O$_8$ is an electrically insulating geometrically frustratedantiferromagnet in which inorganic Mo$_3$O$_{13}$ clusters each behaves as asingle $S = 1/2$ unit, with the clusters arranged on a two-dimensionaltriangular lattice. Prior results have shown that LiZn$_2$Mo$_3$O$_8$ does notexhibit static magnetic order down to at least $T = 0.05\,K$, and insteadpossesses a valence bond ground state. Here, we show that LiZn$_2$Mo$_3$O$_8$can be hole doped by oxidation with $\mathrm{I}_2$ and subsequent removal of$\mathrm{Zn}^{2+}$ cations to access the entire range of electron count, fromone to zero unpaired electrons per site on the triangular lattice. Contrary toexpectations, no metallic state is induced; instead, the primary effect is tosuppress the number of sites contributing to the condensed valence-bond state.Further, diffraction and pair-distribution function analysis show no evidencefor local Jahn-Teller distortions or other deviations from the parent trigonalsymmetry as a function of doping or temperature. Taken together, the data anddensity functional theory calculations indicate that removal of electrons fromthe magnetic layers favors Anderson localization of the resulting hole and anincrease in the electrical band-gap over the formation of a metallic andsuperconducting state. These results put strong constraints on the chemicalconditions necessary to realize metallic states from parent insulatinggeometrically frustrated antiferromagnets.

Electronic tunability of the frustrated triangular-lattice cluster magnet LiZn$_{2-x}$Mo$_3$O$_8$