Abstract
Muon spin relaxation $(\ensuremath{\mu}\text{SR})$ and nuclear magnetic resonance experiments revealed that the spin-singlet state with an excitation gap of $\ensuremath{\sim}200\text{ }\text{K}$ is realized from $S=1/2\text{ }{\text{Nb}}_{4}$ tetrahedral clusters in a cluster Mott insulator ${\text{GaNb}}_{4}{\text{S}}_{8}$. The intercluster cooperative phenomenon to the singlet state at ${T}_{\text{S}}=32\text{ }\text{k}$ is triggered by intracluster Jahn-Teller type structural instability developed from $\ensuremath{\sim}3{T}_{\text{S}}$. Referring to the lattice symmetry, the formation of ${\text{Nb}}_{8}$ octamer (${\text{Nb}}_{4}{\text{-Nb}}_{4}$ bond) is suggested.
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