The rare-earth metal hydrides with clathrate structures have been highly attractive because of their promising high-Tc superconductivity at high pressure. Recently, cerium hydride CeH9 composed of Ce-encapsulated clathrate H cages was synthesized at much lower pressures of 80−100 GPa, compared to other experimentally synthesized rare-earth hydrides such as LaH10 and YH6. Based on density-functional theory calculations, we find that the Ce 5p semicore and 4f/5d valence states strongly hybridize with the H 1s state, while a transfer of electrons occurs from Ce to H atoms. Further, we reveal that the delocalized nature of Ce 4f electrons plays an important role in the chemical precompression of clathrate H cages. Our findings not only suggest that the bonding nature between the Ce atoms and H cages is characterized as a mixture of ionic and covalent, but also have important implications for understanding the origin of enhanced chemical precompression that results in the lower pressures required for the synthesis of CeH9.
@article{arxiv.2007.02073,
title = {Origin of enhanced chemical precompression in cerium hydride CeH$_{9}$},
author = {Hyunsoo Jeon and Chongze Wang and Seho Yi and Jun-Hyung Cho},
journal= {arXiv preprint arXiv:2007.02073},
year = {2020}
}