2024-03-28T09:46:39Zhttps://eprints.lib.hokudai.ac.jp/dspace-oai/requestoai:eprints.lib.hokudai.ac.jp:2115/812712022-11-17T02:08:08Zhdl_2115_20059hdl_2115_151Surface Oxygen Vacancy Formation Energy Calculations in 34 Orientations of beta-Ga2O3 and theta-Al2O3Hinuma, Yoyo1000040403951Kamachi, TakashiHamamoto, NobutsuguTakao, Motoshi1000080775388Toyao, Takashi1000060324000Shimizu, Ken-ichiopen accessThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry C, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.jpcc.0c00994 .431Computational exploration of previously unknown reactive sites is a powerful strategy for the emergence of new catalytic reactions. Exotic surfaces can be theoretically investigated, but there are very few, if any, computational models of high-index orientations that consider the reconstruction of the surface. A workflow to efficiently obtain a set of accessible terminations by removing those that are metastable against macroscopic facet formation and by comparing cleaved surfaces and surfaces suggested by a genetic algorithm (GA) for promising orientations is proposed and demonstrated using 34 orientations of beta-Ga2O3 and theta-Al2O3. Seven and six terminations considered to be experimentally accessible are found for beta-Ga2O3 and theta-Al2O3, respectively, where the highest surface energy was roughly twice that of the lowest. The lowest surface 0 vacancy formation - energies (E-Ovac) among accessible surfaces are 3.04 and 5.46 eV in the (101) and (20 (1) over bar) terminations for beta-Ga2O3 and theta-Al2O3, respectively, where the decreases in E-Ovac, from the most stable surface are 1.32 and 1.11 eV, respectively. The E-Ovac in accessible surfaces showed a good correlation with the descriptors of the local coordination environment, suggesting that exploiting surface O in an unfavorable environment in an accessible termination would enhance O-vacancy-related catalyst performance even in materials that do not show reactivity on the most stable surface.American Chemical Society2020-05-14engjournal articleAMhttp://hdl.handle.net/2115/81271https://doi.org/10.1021/acs.jpcc.0c009941932-7447Journal of physical chemistry c124191050910522https://eprints.lib.hokudai.ac.jp/dspace/bitstream/2115/81271/1/Galia_alumina_surface_for%20HUSCAP.pdfapplication/pdf972.07 KB2020-05-14