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

Strong spin–orbit coupling lifts the degeneracy of t 2g orbitals in 5 d transition-metal systems, leaving a Kramers doublet and quartet with effective angular momentum of J eff = 1/2 and 3/2, respectively. These spin–orbit entangled states can host exotic quantum phases such as topological Mott state, unconventional superconductivity, and quantum spin liquid. The lacunar spinel GaTa 4 Se 8 was theoretically predicted to form the molecular J eff = 3/2 ground state. Experimental verification of its existence is an important first step to exploring the consequences of the J eff = 3/2 state. Here, we report direct experimental evidence of the J eff = 3/2 state in GaTa 4 Se 8 by means of excitation spectra of resonant inelastic X-ray scattering at the Ta L 3 and L 2 edges. We find that the excitations involving the J eff = 1/2 molecular orbital are absent only at the Ta L 2 edge, manifesting the realization of the molecular J eff = 3/2 ground state in GaTa 4 Se 8 . The strong interaction between electron spin and orbital degrees of freedom in 5 d oxides can lead to exotic electronic ground states. Here the authors use resonant inelastic X-ray scattering to demonstrate that the theoretically proposed J eff = 3/2 state is realised in GaTa 4 Se 8 .