Ab initio study of metastable occupation of tetrahedral sites in palladium hydrides and its impact on superconductivity
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Physical Review B 107(2) : (2023) // Article ID 024504,
A recent experimental work on palladium hydrides suggested that metastable structures with hydrogen atoms occupying tetrahedral sites could lead to superconductivity above 50 K, a huge increase compared to the 9 K critical temperature of the stable structure with all hydrogen atoms occupying octahedral sites. By generating many structures with hydrogen atoms randomly occupying the octahedral and tetrahedral sites of the face-centered-cubic lattice and calculating their energy at different theoretical levels from first principles, we determine that metastable structures with partial or full occupation of tetrahedral sites are possible, even when the ionic quantum zero-point energy and anharmonicity are included in the calculations. Anharmonicity is crucial in palladium hydrides when hydrogen atoms occupy octahedral sites and, in fact, makes the structure with full octahedral occupation the ground state. Despite the metastable existence of structures with full or partial tetrahedral site occupation, the superconducting critical temperature is reduced with the number of tetrahedral sites occupied. Our calculations discard that the occupation of tetrahedral sites can increase the critical temperature in palladium hydrides.