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Abstract High entropy oxides (HEOs) have garnered much interest due to their available high degree of tunability. Here, we study the local structure of (MgNiCuCoZn)0.167(MnCr)0.083O, a composition based on the parent HEO (MgNiCuCoZn)0.2O. We synthesized a series of thin films via pulsed laser deposition at incremental oxygen partial pressures. X‐ray diffraction shows lattice parameters to decrease with increased pO2 pressures until the onset of phase separation. X‐ray absorption fine structure shows that specific atomic species in the composition dictate the global structure of the material as Cr, Co, and Mn shift to energetically favorable coordination with increasing pressure. Transmission electron microscopy analysis on a lower‐pressure sample exhibits a rock salt structure, but the higher‐pressure sample reveals reflections reminiscent of the spinel structure. In all, these findings give a more complete picture of how (MgNiCuCoZn)0.167(MnCr)0.083O forms with varying initial conditions and advances fundamental knowledge of cation behavior in high entropy oxides.more » « lessFree, publicly-accessible full text available February 1, 2026
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Min, Lujin; Barber, John P; Wang, Yu; Gayathri_Ayyagari, Sai Venkata; Niculescu, Gabriela E; Krysko, Evan; Bejger, Gerald R; Miao, Leixin; Lee, Seng Huat; Zhang, Qiang; et al (, Journal of the American Chemical Society)
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Kotsonis, George N; Almishal, Saeed_S I; Miao, Leixin; Caucci, Mary Kathleen; Bejger, Gerald R; Ayyagari, Sai_Venkata Gayathri; Valentine, Tyler W; Yang, Billy E; Sinnott, Susan B; Rost, Christina M; et al (, Applied Physics Letters)The prototype high-entropy oxide (HEO) Y0.2La0.2Ce0.2Pr0.2Sm0.2O2−δ represents a particularly complex class of HEOs with significant anion sublattice entropy. The system takes either a fluorite or bixbyite-type crystal structure, depending on synthesis kinetics and thermal history. Here, we synthesize bulk ceramics and epitaxial thin films of Y0.2La0.2Ce0.2Pr0.2Sm0.2O2−δ and use diffraction to explore crystal symmetry and phase. Thin films exhibit the high symmetry fluorite phase, while bulk ceramics adopt the lower symmetry bixbyite phase. The difference in chemical ordering and observed symmetry between vapor-deposited and reactively sintered specimens suggests that synthesis kinetics can influence accessible local atomic configurations, i.e., the high kinetic energy adatoms quench in a higher-effective temperature, and thus higher symmetry structure with more configurational entropy. More generally, this demonstration shows that recovered HEO specimens can exhibit appreciably different local configurations depending on synthesis kinetics, with potential ramifications on macroscopic physical properties.more » « less
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