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 GaTa₄Se₈ using resonant inelastic x-ray scattering (RIXS) at the Ta L₃ edge. Electrons are fully delocalized over Ta₄ tetrahedra, forming quasimolecular Jₜₑₜ=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.
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Magnaterra et al. (2024) studied this question.
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