Defect levels and hyperfine constants of hydrogen in beryllium oxide from hybrid-functional calculations and muonium spectroscopy
authors Marinopoulos, AG; Vilao, RC; Vieira, RBL; Alberto, HV; Gil, JM; Yakushev, MV; Scheuermann, R; Goko, T
nationality International
journal PHILOSOPHICAL MAGAZINE
author keywords Ab initio calculations; oxides; hydrogen; muonium; hyperfine constants
keywords INITIO MOLECULAR-DYNAMICS; AUGMENTED-WAVE METHOD; 1ST-PRINCIPLES CALCULATIONS; ELECTRONIC-PROPERTIES; WURTZITE BEO; SEMICONDUCTORS; STATES; RELIABILITY; TRANSITION; PARAMETERS
abstract The atomistic and electronic structures of isolated hydrogen states in BeO were studied by ab initio calculations and muonium spectroscopy (mu 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 alkalineearth 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 minimumenergy 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 elongatedbond 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 H0 configuration is dominated by an isotropic hyperfine interaction with a magnitude very close to the vacuum value, a finding corroborated by the mu SR-spectroscopy data.
publisher TAYLOR & FRANCIS LTD
issn 1478-6435
year published 2017
volume 97
issue 24
beginning page 2108
ending page 2128
digital object identifier (doi) 10.1080/14786435.2017.1328133
subject category 21
unique article identifier Materials Science; Metallurgy & Metallurgical Engineering; Physics