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LiVO$_2$ is a model system of the valence bond solid (VBS) in $3d^2$triangular lattice. The origin of the VBS formation has remained controversial.We investigate the microscopic mechanism by elucidating the $d$ orbitalcharacter via on-site $^{51}$V NMR measurements in a single crystal up to 550 Kacross a structural transition temperature $T_c$. The Knight shift, $K$, andnuclear quadrupole frequency, $\delta \nu$, show that the 3d orbital with localtrigonal symmetry are reconstructed into a $d_{yz}d_{zx}$ orbital order below$T_c$. Together with the NMR spectra with three-fold rotational symmetry, weconfirm a vanadium trimerization with $d$-$d$ $\sigma$ bonds. The Knight shiftextracts the large Van-Vleck orbital susceptibility, $\chi^{\rm VV} = 3.6\times 10^{-4}$, in a paramagnetic state above $T_c$, which is comparable tothe spin susceptibility. The results suggest that orbitally induced Peierlstransition in the proximity of the frustrated itinerant state is the dominantdriving force of the trimerization transition.

Orbital reformation with vanadium trimerization in $d^2$ triangular lattice LiVO$_2$ revealed by $^{51}$V NMR