We present a comprehensive study of the inhomogeneous mixed-valence compound, EuPd3S4, by electrical transport, X-ray diffraction, time-domain 151Eu synchrotron Mössbauer spectroscopy, and X-ray absorption spectroscopy measurements under high pressure. Electrical transport measurements show that the antiferromagnetic ordering temperature, TN, increases rapidly from 2.8 K at ambient pressure to 23.5 K at ∼19 GPa and plateaus between ∼19 and ∼29 GPa after which no anomaly associated with TN is detected. A pressure-induced first-order structural transition from cubic to tetragonal is observed, with a rather broad coexistence region (∼20 GPa to ∼30 GPa) that corresponds to the TN plateau. Mössbauer spectroscopy measurements show a clear valence transition from approximately 50:50 Eu2+:Eu3+ to fully Eu3+ at ∼28 GPa, consistent with the vanishing of the magnetic order at the same pressure. X-ray absorption data show a transition to a fully trivalent state at a similar pressure. Our results show that pressure first greatly enhances TN, most likely via enhanced hybridization between the Eu 4f states and the conduction band, and then, second, causes a structural phase transition that coincides with the conversion of the europium to a fully trivalent state.
CITATION STYLE
Huyan, S., Ryan, D. H., Slade, T. J., Lavina, B., Jose, G., Wang, H., … Canfield, P. C. (2023). Strong enhancement of magnetic ordering temperature and structural/valence transitions in EuPd3S4 under high pressure. Proceedings of the National Academy of Sciences of the United States of America, 120(52). https://doi.org/10.1073/pnas.2310779120
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