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Title: Thickness-dependent energetics for Pb adatoms on low-index Pb nanofilm surfaces: First-principles calculations

Abstract

Adsorption, interaction, and diffusion of adatoms on surfaces control growth and relaxation of epitaxial nanostructures and nanofilms. Previous reports of key diffusion barriers for Pb diffusion on low-index Pb surfaces are limited in scope and accuracy. Thus, we apply density functional theory (DFT) to calculate the adsorption and diffusion energetics for a Pb adatom on Pb(111), Pb(100), and Pb(110) nanofilms with different thicknesses. We find that these quantities exhibit damped oscillatory variation with increasing film thickness. For Pb(111) films, energetics along the minimum energy path for Pb adatom diffusion between adjacent fcc and hcp sites varies significantly with film thickness, its form differing from other metal-on-metal(111) systems. For Pb(111) and Pb(100) nanofilms, diffusion barriers obtained for both adatom hopping and exchange mechanism differ significantly from previous DFT results. Hopping is favored over exchange for Pb(111), and the opposite applies for Pb(100). For Pb(110) nanofilms, Pb adatom hopping over an in-channel bridge is most facile, then in-channel exchange, then cross-channel exchange, with cross-channel hopping least favorable. We also assess lateral Pb adatom interactions, and characterize island nucleation during deposition on Pb(111).

Authors:
 [1];  [1];  [2];  [3];  [4];  [5];  [5]
  1. Southern Univ. of Science and Technology, Shenzhen, Guangdong (China). Dept. of Physics
  2. Indian Inst. of Technology, Kanpur (India). Dept. of Chemical Engineering; Indian Ist. of Technology, Kanpur (India). Material Science Programme
  3. Beihang Univ., Beijing (China). Dept. of Physics; Beihang Univ., Beijing (China). Beijing Key Lab. of Advanced Nuclear Materials and Physics
  4. Univ. of Utah, Salt Lake City, UT (United States). Dept. of Materials Science and Engineering
  5. Iowa State Univ., Ames, IA (United States). Dept. of Physics and Astronomy; Iowa State Univ., Ames, IA (United States). Ames-Lab. - U.S. Dept. of Energy
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1544356
Alternate Identifier(s):
OSTI ID: 1407439
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 96; Journal Issue: 20; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Li, Wei, Huang, Li, Pala, Raj Ganesh S., Lu, Guang-Hong, Liu, Feng, Evans, James W., and Han, Yong. Thickness-dependent energetics for Pb adatoms on low-index Pb nanofilm surfaces: First-principles calculations. United States: N. p., 2017. Web. doi:10.1103/PhysRevB.96.205409.
Li, Wei, Huang, Li, Pala, Raj Ganesh S., Lu, Guang-Hong, Liu, Feng, Evans, James W., & Han, Yong. Thickness-dependent energetics for Pb adatoms on low-index Pb nanofilm surfaces: First-principles calculations. United States. doi:10.1103/PhysRevB.96.205409.
Li, Wei, Huang, Li, Pala, Raj Ganesh S., Lu, Guang-Hong, Liu, Feng, Evans, James W., and Han, Yong. Mon . "Thickness-dependent energetics for Pb adatoms on low-index Pb nanofilm surfaces: First-principles calculations". United States. doi:10.1103/PhysRevB.96.205409. https://www.osti.gov/servlets/purl/1544356.
@article{osti_1544356,
title = {Thickness-dependent energetics for Pb adatoms on low-index Pb nanofilm surfaces: First-principles calculations},
author = {Li, Wei and Huang, Li and Pala, Raj Ganesh S. and Lu, Guang-Hong and Liu, Feng and Evans, James W. and Han, Yong},
abstractNote = {Adsorption, interaction, and diffusion of adatoms on surfaces control growth and relaxation of epitaxial nanostructures and nanofilms. Previous reports of key diffusion barriers for Pb diffusion on low-index Pb surfaces are limited in scope and accuracy. Thus, we apply density functional theory (DFT) to calculate the adsorption and diffusion energetics for a Pb adatom on Pb(111), Pb(100), and Pb(110) nanofilms with different thicknesses. We find that these quantities exhibit damped oscillatory variation with increasing film thickness. For Pb(111) films, energetics along the minimum energy path for Pb adatom diffusion between adjacent fcc and hcp sites varies significantly with film thickness, its form differing from other metal-on-metal(111) systems. For Pb(111) and Pb(100) nanofilms, diffusion barriers obtained for both adatom hopping and exchange mechanism differ significantly from previous DFT results. Hopping is favored over exchange for Pb(111), and the opposite applies for Pb(100). For Pb(110) nanofilms, Pb adatom hopping over an in-channel bridge is most facile, then in-channel exchange, then cross-channel exchange, with cross-channel hopping least favorable. We also assess lateral Pb adatom interactions, and characterize island nucleation during deposition on Pb(111).},
doi = {10.1103/PhysRevB.96.205409},
journal = {Physical Review B},
number = 20,
volume = 96,
place = {United States},
year = {2017},
month = {11}
}

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Figures / Tables:

TABLE I TABLE I: Lattice constant a (in nm), cohesive energymore » $E$c (in eV/atom), bulk modulus $B$ (in GPa), and relaxed monovacancy formation energy $E$$^{1v}_{f}$ (in eV) of bulk fcc Pb crystal from our PBE and PBEsol calculations, compared with experimental values.« less

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