Quasimolecular J_{tet}=3/2 Moments in the Cluster Mott Insulator GaTa_{4}Se_{8}.

Quasimolecular orbitals in cluster Mott insulators provide a route to tailor exchange interactions, which may yield novel quantum phases of matter. We demonstrate the cluster Mott character of the lacunar spinel GaTa_{4}Se_{8} using resonant inelastic x-ray scattering (RIXS) at the Ta L_{3} edge. Electrons are fully delocalized over Ta_{4} tetrahedra, forming quasimolecular J_{tet}=3/2 moments. The modulation of the RIXS intensity as function of the transferred momentum q allows us to determine the cluster wave function, which depends on competing intracluster hopping terms that mix states with different character. This mixed wave function is decisive for the macroscopic properties since it affects intercluster hopping and exchange interactions and furthermore renormalizes the effective spin-orbit coupling constant. The versatile wave function, tunable via intracluster hopping, opens a new perspective on the large family of lacunar spinels and cluster Mott insulators in general.