Energy barriers for Pb adatom diffusion on stepped ultrathin Pb(111) quantum nanofilms: First-principles calculations
Abstract
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 aremore »
- Authors:
-
[1];
[1];
- 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
- Publication Date:
- Research Org.:
- Ames Lab., Ames, IA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1574814
- Report Number(s):
- IS-J-10089
Journal ID: ISSN 2469-9950; PRBMDO; TRN: US2100045
- Grant/Contract Number:
- CHE-1507223; AC02-07CH11358; FG02-04ER46148
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 100; Journal Issue: 19; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Han, Yong, Evans, James W., and Liu, Feng. Energy barriers for Pb adatom diffusion on stepped ultrathin Pb(111) quantum nanofilms: First-principles calculations. United States: N. p., 2019.
Web. doi:10.1103/PhysRevB.100.195405.
Han, Yong, Evans, James W., & Liu, Feng. Energy barriers for Pb adatom diffusion on stepped ultrathin Pb(111) quantum nanofilms: First-principles calculations. United States. https://doi.org/10.1103/PhysRevB.100.195405
Han, Yong, Evans, James W., and Liu, Feng. Tue .
"Energy barriers for Pb adatom diffusion on stepped ultrathin Pb(111) quantum nanofilms: First-principles calculations". United States. https://doi.org/10.1103/PhysRevB.100.195405. https://www.osti.gov/servlets/purl/1574814.
@article{osti_1574814,
title = {Energy barriers for Pb adatom diffusion on stepped ultrathin Pb(111) quantum nanofilms: First-principles calculations},
author = {Han, Yong and Evans, James W. and Liu, Feng},
abstractNote = {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.},
doi = {10.1103/PhysRevB.100.195405},
journal = {Physical Review B},
number = 19,
volume = 100,
place = {United States},
year = {Tue Nov 05 00:00:00 EST 2019},
month = {Tue Nov 05 00:00:00 EST 2019}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 4 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Thickness-dependent energetics for Pb adatoms on low-index Pb nanofilm surfaces: First-principles calculations
journal, November 2017
- Li, Wei; Huang, Li; Pala, Raj Ganesh S.
- Physical Review B, Vol. 96, Issue 20
Height-dependent barriers and nucleation in quantum size effect growth
journal, October 2008
- Kuntová, Z.; Tringides, M. C.; Chvoj, Z.
- Physical Review B, Vol. 78, Issue 15
Quantum Size Effect on Adatom Surface Diffusion
journal, December 2006
- Ma, Li-Ying; Tang, Lin; Guan, Ze-Lei
- Physical Review Letters, Vol. 97, Issue 26
Experimental observation of quantum oscillation of surface chemical reactivities
journal, May 2007
- Ma, X.; Jiang, P.; Qi, Y.
- Proceedings of the National Academy of Sciences, Vol. 104, Issue 22
Deeper insight into phase relations in ultrathin Pb films
journal, September 2015
- Liu, Ro-Ya; Huang, Angus; Huang, Chien-Chung
- Physical Review B, Vol. 92, Issue 11
Quantum Size Effect on the Diffusion Barriers and Growth Morphology of
journal, June 2006
- Chan, T. -L.; Wang, C. Z.; Hupalo, M.
- Physical Review Letters, Vol. 96, Issue 22
Atomic View of Surface Self‐Diffusion: Tungsten on Tungsten
journal, February 1966
- Ehrlich, Gert; Hudda, F. G.
- The Journal of Chemical Physics, Vol. 44, Issue 3
Phase Relations Associated with One-Dimensional Shell Effects in Thin Metal Films
journal, June 2009
- Miller, T.; Chou, M. Y.; Chiang, T. -C.
- Physical Review Letters, Vol. 102, Issue 23
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Bilayer-ring second-layer nucleation morphology in
journal, May 2007
- Kuntova, Z.; Hupalo, M.; Chvoj, Z.
- Physical Review B, Vol. 75, Issue 20
Band Structure and Oscillatory Electron-Phonon Coupling of Pb Thin Films Determined by Atomic-Layer-Resolved Quantum-Well States
journal, August 2005
- Zhang, Yan-Feng; Jia, Jin-Feng; Han, Tie-Zhu
- Physical Review Letters, Vol. 95, Issue 9
A theory of thin metal films: electron density, potentials and work function
journal, May 1976
- Schulte, F. K.
- Surface Science, Vol. 55, Issue 2
Evidence for Quantum Size Effects Observed by Helium Atom Scattering during the Growth of Pb on Cu(111)
journal, October 1989
- Hinch, B. J.; Koziol, C.; Toennies, J. P.
- Europhysics Letters (EPL), Vol. 10, Issue 4
Alternating Layer and Island Growth of Pb on Si by Spontaneous Quantum Phase Separation
journal, February 2003
- Hong, Hawoong; Wei, C. -M.; Chou, M. Y.
- Physical Review Letters, Vol. 90, Issue 7
Step Motion on Crystal Surfaces
journal, September 1966
- Schwoebel, Richard L.; Shipsey, Edward J.
- Journal of Applied Physics, Vol. 37, Issue 10
Morphological evolution during epitaxial thin film growth: Formation of 2D islands and 3D mounds
journal, April 2006
- Evans, J. W.; Thiel, P. A.; Bartelt, M. C.
- Surface Science Reports, Vol. 61, Issue 1-2
Thermal Stability and Electronic Structure of Atomically Uniform Pb Films on Si(111)
journal, July 2004
- Upton, M. H.; Wei, C. M.; Chou, M. Y.
- Physical Review Letters, Vol. 93, Issue 2
Non-classical kinetics processes and morphologies in QSE driven growth in Pb/Si(111)
journal, October 2006
- Kuntova, Z.; Hupalo, M.; Chvoj, Z.
- Surface Science, Vol. 600, Issue 20
Theory of quantum size effects in thin Pb(111) films
journal, December 2002
- Wei, C. M.; Chou, M. Y.
- Physical Review B, Vol. 66, Issue 23
Permeability and kinetic coefficients for mesoscale BCF surface step dynamics: Discrete two-dimensional deposition-diffusion equation analysis
journal, April 2016
- Zhao, Renjie; Evans, James W.; Oliveira, Tiago J.
- Physical Review B, Vol. 93, Issue 16
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000
- Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
- The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
Reshaping, Intermixing, and Coarsening for Metallic Nanocrystals: Nonequilibrium Statistical Mechanical and Coarse-Grained Modeling
journal, October 2018
- Lai, King C.; Han, Yong; Spurgeon, Peter
- Chemical Reviews, Vol. 119, Issue 11
Level set simulation of directed self-assembly during epitaxial growth
journal, November 2006
- Niu, X.; Vardavas, R.; Caflisch, R. E.
- Physical Review B, Vol. 74, Issue 19
Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points
journal, December 2000
- Henkelman, Graeme; Jónsson, Hannes
- The Journal of Chemical Physics, Vol. 113, Issue 22
Quantum Beating Patterns Observed in the Energetics of Pb Film Nanostructures
journal, July 2004
- Czoschke, P.; Hong, Hawoong; Basile, L.
- Physical Review Letters, Vol. 93, Issue 3
Height-dependent nucleation and ideal layer by layer growth in Pb/Pb(111)/Si(111)
journal, November 2008
- Binz, S. M.; Hupalo, M.; Tringides, M. C.
- Physical Review B, Vol. 78, Issue 19
Quantum size effects in metal nanofilms: Comparison of an electron-gas model and density functional theory calculations
journal, October 2009
- Han, Yong; Liu, Da-Jiang
- Physical Review B, Vol. 80, Issue 15
Controlling nucleation rates in nanostructures with electron confinement
journal, March 2010
- Kuntová, Z.; Tringides, M. C.; Binz, S. M.
- Surface Science, Vol. 604, Issue 5-6
Quantum size effects in quasi-free-standing Pb layers
journal, April 2007
- Dil, J. H.; Kampen, T. U.; Hülsen, B.
- Physical Review B, Vol. 75, Issue 16
Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets
journal, May 2021
- Chen, Ruyi; Cui, Qirui; Liao, Liyang
- Nature Communications, Vol. 12, Issue 1