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Defect levels and hyperfine constants of hydrogen in beryllium oxide from hybrid-functional calculations and muonium spectroscopy

Authors: AG Marinopoulos, RC Vilão, RBL Vieira, HV Alberto, JM Gil, MV Yakushev, R Scheuermann, T Goko

Ref.: Philosophical Magazine 97, 2108-2128 (2017)

Abstract: The atomistic and electronic structures of isolated hydrogen states in BeO were studied by ab initio calculations and muonium spectroscopy (SR). Whereas standard density-functional theory with a semi-local GGA functional led to a detailed probing of all possible minimum-energy configurations of hydrogen further calculations with the hybrid HSE06 functional provided improved properties avoiding band-gap and self-interaction errors. Similarly to earlier findings for the other wide-gap alkaline-earth oxide, MgO, hydrogen in BeO is also predicted to be an amphoteric defect with the pinning level, E(+/-), positioned in the mid-gap region. Both donor and acceptor levels were found too deep in the gap to allow for hydrogen to act as a source of free carriers. Whereas, hydrogen in its positively-charged state, H+, adopts exclusively hydroxide-bond OH configurations, H0 and H- instead show a preference to occupy cage-like interstitial sites in the lattice. H0 in particular displays a multitude of minimum-energy configurations: its lowest-energy ground state resembles closely a trapped-atom state with a nearly spherical spin-density profile. In contrast to the strongly ionic MgO, H0 in BeO was further found to stabilise in additional higher-energy elongated-bond OH configurations whose existence should be traced to a partial covalent character of the Be–O bonding. Calculations of the proton-electron hyperfine coupling for all H0 states showed that the ground-state interstitial configuration is dominated by an isotropic hyperfine interaction with a magnitude very close to the vacuum value, a finding corroborated by the muSR-spectroscopy data.

DOI: https://doi.org/10.1080/14786435.2017.1328133