Energy barriers for Pb adatom diffusion on stepped ultrathin Pb(111) quantum nanofilms: First-principles calculations

Han, Yong; Evans, James W.; Liu, Feng

doi:10.1103/PhysRevB.100.195405

Title: Energy barriers for Pb adatom diffusion on stepped ultrathin Pb(111) quantum nanofilms: First-principles calculations

Journal Article · Tue Nov 05 00:00:00 EST 2019 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.100.195405· OSTI ID:1574814

^[1];

^[1]; Liu, Feng ^[2]

Iowa State Univ., Ames, IA (United States). Dept. of Physics and Astronomy; Ames Lab., and Iowa State Univ., Ames, IA (United States)
Univ. of Utah, Salt Lake City, UT (United States). Dept. of Materials Science and Engineering

Various properties of Pb(111) nanofilms, prototypical quantum films, have been studied extensively. However, key ab initio-level energy barriers for Pb adatom diffusion on stepped Pb(111) nanofilm surfaces are still not available. Using first-principles density functional theory, we calculate these barriers for films with thicknesses of few monolayers (ML). We find that two-atom exchange is always much more favorable than direct hopping to cross A- or B-type steps. Ehrlich-Schwoebel (ES) barriers for downward transport to a higher-coordination step-edge site depend strongly on the film thickness. For such transport from 2- to 1-ML terraces, or from 4- to 3-ML terraces, there is no an ES barrier, but large ES barriers of more than 100 meV are found from 3- to 2-ML terraces. We also obtain the barriers for diffusion along the step edges and find that these step-edge barriers are significantly larger than terrace diffusion barriers. In addition, we analyze energetics for diffusion on the top flat surface of a nanofilm supported on a vicinal surface, and thus having underlying buried or ghost steps. We quantify the tilted potential energy surface in both ghost A- and B-step regions separating 2- and 3-ML (as well as 3- and 4-ML) terraces. Finally, consequences are discussed for the growth kinetics of supported Pb nanofilms, where the support does not strongly affect electronic states within the film.

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Research Organization:: Ames Lab., Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: CHE-1507223; AC02-07CH11358; FG02-04ER46148

OSTI ID:: 1574814

Report Number(s):: IS-J-10089; PRBMDO; TRN: US2100045

Journal Information:: Physical Review B, Vol. 100, Issue 19; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 4 works

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