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Strong spin-orbit coupling lifts the degeneracy of t2g orbitals in 5dtransition-metal systems, leaving a Kramers doublet and quartet with effectiveangular momentum of Jeff = 1/2 and 3/2, respectively. These spin-orbitentangled states can host exotic quantum phases such as topological Mott state,unconventional superconductivity, and quantum spin liquid. The lacunar spinelGaTa4Se8 was theoretically predicted to form the molecular Jeff = 3/2 groundstate. Experimental verification of its existence is an important first step toexploring the consequences of the Jeff = 3/2 state. Here, we report directexperimental evidence of the Jeff = 3/2 state in GaTa4Se8 by means ofexcitation spectra of resonant inelastic x-rays scattering at the Ta L3 and L2edges. We found that the excitations involving the Jeff = 1/2 molecular orbitalwere suppressed only at the Ta L2 edge, manifesting the realization of themolecular Jeff = 3/2 ground state in GaTa4Se8.

Direct experimental observation of the molecular Jeff=3/2 ground state in the lacunar spinel GaTa4Se8