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We present a comprehensive study of the mixed valent compound, EuPd3S4, byelectrical transport, X-ray diffraction, time-domain 151Eu synchrotronM\"ossbauer spectroscopy, and X-ray absorption spectroscopy measurements underhigh pressure. The electrical transport measurements show that theantiferromagnetic ordering temperature, TN, increases rapidly from 2.8 K atambient pressure to 23.5 K at ~19 GPa and plateaus between ~19 and ~29 GPaafter which no anomaly associated with TN is detected. A pressure-induced firstorder structural transition from cubic to tetragonal is observed, with a ratherbroad coexistence region (~20 GPa to ~32 GPa) that corresponds to the TNplateau. M\"ossbauer spectroscopy measurements show a clear valence transitionfrom approximately 50:50 Eu2+:Eu3+ to fully Eu3+ at ~28 GPa, consistent withthe vanishing of the magnetic order at the same pressure. X-ray absorption datashow a transition to a fully trivalent state at a similar pressure. Our resultsshow that pressure first greatly enhances TN, most likely via enhancedhybridization between the Eu 4f states and the conduction band, and then,second, causes a structural phase transition that coincides with the conversionof the europium to a fully trivalent state.

Strong enhancement of magnetic ordering temperature and structural/valence transitions in EuPd3S4 under high pressure