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The spin-orbit entangled (SOE) Jeff-state has been a fertile ground to studynovel quantum phenomena. Contrary to the conventional weakly correlatedJeff=1/2 state of 4d and 5d transition metal compounds, the ground state ofCuAl2O4 hosts a Jeff=1/2 state with a strong correlation of Coulomb U. Here, wereport that surprisingly Cu2+ ions of CuAl2O4 overcome the otherwise usuallystrong Jahn-Teller distortion and instead stabilize the SOE state, although thecuprate has relatively small spin-orbit coupling. From the x-ray absorptionspectroscopy and high-pressure x-ray diffraction studies, we obtained definiteevidence of the Jeff=1/2 state with a cubic lattice at ambient pressure. Wealso found the pressure-induced structural transition to a compressedtetragonal lattice consisting of the spin-only S=1/2 state for pressure higherthan Pc=8 GPa. This phase transition from the Mott insulating Jeff=1/2 to theS=1/2 states is a unique phenomenon and has not been reported before. Our studyoffers a rare example of the SOE Jeff-state under strong electron correlationand its pressure-induced transition to the S=1/2 state.

Pressure-induced transition from Jeff=1/2 to S=1/2 states in CuAl2O4