Materials Chemistry

Hydride superconductor structures of LaH10, EuH9, and UH8 rationalized by electron counting and Jahn-Teller distortions in a covalent cluster model



The superconducting hydrides LaH10, EuH9 and UH8 are studied using chemically intuitive bonding analysis of periodic and molecular models. We find trends in the crystallographic and electronic structures of the materials by focusing on chemically meaningful building blocks in the H sublattice. Atomic charge calculations, using two complementary techniques, allow us to assign oxidation states to the metals and divide the H sublattice into neutral and anionic components. Cubic [H8]q- clusters are an important structural motif, and molecular orbital analysis of this cluster in isolation shows the crystal structures to be consistent with our oxidation state assignments. Crystal orbital hamilton population analysis confirms the applicability of the cluster model to the periodic electronic structure. A Jahn-Teller distortion predicted by MO analysis rationalises the distortion observed in EuH9. Additionally, the performance of analytical methods at high pressures are tested and recommendations for future studies are given. These results demonstrate the value of simple bonding models in rationalizing chemical structures under extreme conditions.


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Supplementary material

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Supporting information
Method testing results and additional electronic structure figures
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Geometry archive
Zip archive of all DFT-optimized geometries used in this study