Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

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]
+ Show Author Affiliations
  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.
Copy to clipboard
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. https://doi.org/10.1103/PhysRevB.96.205409
Copy to clipboard
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. https://doi.org/10.1103/PhysRevB.96.205409. https://www.osti.gov/servlets/purl/1544356.
Copy to clipboard
@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 = {Mon Nov 06 00:00:00 EST 2017},
month = {Mon Nov 06 00:00:00 EST 2017}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1103/PhysRevB.96.205409
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 13 works
Citation information provided by
Web of Science

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
All figures and tables (17 total)
Save / Share:
Export Metadata
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:

Fabricating artificial nanowells with tunable size and shape by using scanning tunneling microscopy
journal, September 2006

  • Li, Shao-Chun; Jia, Jin-Feng; Ma, Xucun
  • Applied Physics Letters, Vol. 89, Issue 12
  • DOI: 10.1063/1.2355461

Competing Classical and Quantum Effects in Shape Relaxation of a Metallic Island
journal, November 2002

Projector augmented-wave method
journal, December 1994

Fermi surface of lead under homogeneous strain
journal, May 1981

Ab initio calculations of energies and self-diffusion on flat and stepped surfaces of Al and their implications on crystal growth
journal, February 1996

Quantum Size Effects on the Perpendicular Upper Critical Field in Ultrathin Lead Films
journal, December 2005

Kinetics measurements of Pb island growth on Si(111)
journal, April 2003

Diffusion of the Cu monomer and dimer on Ag(111): Molecular dynamics simulations and density functional theory calculations
journal, August 2010

  • Hayat, Sardar Sikandar; Alcántara Ortigoza, Marisol; Choudhry, Muhammad A.
  • Physical Review B, Vol. 82, Issue 8
  • DOI: 10.1103/PhysRevB.82.085405

Quantum Size Effect on the Diffusion Barriers and Growth Morphology of Pb / Si ( 111 )
journal, June 2006

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

Bilayer-ring second-layer nucleation morphology in Pb ∕ Si ( 111 ) − 7 × 7
journal, May 2007

Band Structure and Oscillatory Electron-Phonon Coupling of Pb Thin Films Determined by Atomic-Layer-Resolved Quantum-Well States
journal, August 2005

Anomalous phase relations of quantum size effects in ultrathin Pb films on Si(111)
journal, June 2013

Adhesion modulation by quantum size effects in Pb∕Si(111) system
journal, October 2006

  • Han, Tie-Zhu; Dong, Guo-Cai; Shen, Quan-Tong
  • Applied Physics Letters, Vol. 89, Issue 18
  • DOI: 10.1063/1.2382729

Plasticity of single-atom Pb junctions
journal, June 2016

Alternating Layer and Island Growth of Pb on Si by Spontaneous Quantum Phase Separation
journal, February 2003

Ultrafast kinetics in Pb ∕ Si ( 111 ) from the collective spreading of the wetting layer
journal, June 2007

Non-classical kinetics processes and morphologies in QSE driven growth in Pb/Si(111)
journal, October 2006

Growth morphology of Pb films on Ni3Al(111)
journal, March 2014

Exchange processes in the contact formation of Pb electrodes
journal, September 2014

Adatom-induced lateral inhomogeneity of quantum well states in metal multilayers
journal, July 2010

Ab initiomolecular dynamics for liquid metals
journal, January 1993

Mechanisms of atomic diffusion on the flat, stepped, and faceted surfaces of Al(110)
journal, May 2010

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
  • DOI: 10.1063/1.1329672

Diffusion of Cu on Cu surfaces
journal, August 1995

Observation of preferred heights in Pb nanoislands: A quantum size effect
journal, September 2002

  • Otero, Roberto; Vázquez de Parga, Amadeo L.; Miranda, Rodolfo
  • Physical Review B, Vol. 66, Issue 11
  • DOI: 10.1103/PhysRevB.66.115401

Quantum Beating Patterns Observed in the Energetics of Pb Film Nanostructures
journal, July 2004

Correlation between Quantized Electronic States and Oscillatory Thickness Relaxations of 2D Pb Islands on Si(111)-( 7 × 7 ) Surfaces
journal, May 2001

Height-dependent nucleation and ideal layer by layer growth in Pb/Pb(111)/Si(111)
journal, November 2008

Ab Initio Thermodynamics and Kinetics for Coalescence of Two-Dimensional Nanoislands and Nanopits on Metal (100) Surfaces
journal, September 2016

  • Han, Yong; Stoldt, Conrad R.; Thiel, Patricia A.
  • The Journal of Physical Chemistry C, Vol. 120, Issue 38
  • DOI: 10.1021/acs.jpcc.6b07328

Quantum size effect in Pb(100) films: Role of symmetry and implications for film growth
journal, September 2006

Absolute surface free energies of Pb
journal, June 2002

Gate-Controlled Atomic Quantum Switch
journal, September 2004

Oscillatory thermal expansion of Pb thin films modulated by quantum size effects
journal, February 2007

  • Zhang, Yan-Feng; Tang, Zhe; Han, Tie-Zhu
  • Applied Physics Letters, Vol. 90, Issue 9
  • DOI: 10.1063/1.2710223

Ab initio calculations of bulk moduli and comparison with experiment
journal, August 2002

Diffusion path for an Al adatom on Al(001)
journal, August 1990

Quantum stability and reentrant bilayer-by-bilayer growth of atomically smooth Pb films on semiconductor substrates
journal, September 2005

Electronic versus Lattice Match for Metal-Semiconductor Epitaxial Growth: Pb on Ge(111)
journal, August 2011

Conductance of atomic-scale Pb contacts in an electrochemical environment
journal, August 2010

Nanoscale “Quantum” Islands on Metal Substrates: Microscopy Studies and Electronic Structure Analyses
journal, July 2010

  • Han, Yong; Ünal, Bariş; Jing, Dapeng
  • Materials, Vol. 3, Issue 7
  • DOI: 10.3390/ma3073965

Quantum size effects on the work function of metallic thin film nanostructures
journal, July 2010

  • Kim, J.; Qin, S.; Yao, W.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 29
  • DOI: 10.1073/pnas.0915171107

Superconductivity Modulated by Quantum Size Effects
journal, December 2004

Height-dependent barriers and nucleation in quantum size effect growth
journal, October 2008

Quantum Size Effect on Adatom Surface Diffusion
journal, December 2006

Deeper insight into phase relations in ultrathin Pb films
journal, September 2015

Quantum size effect in Pb(100) films: Critical role of crystal band structure
journal, May 2007

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Phase Relations Associated with One-Dimensional Shell Effects in Thin Metal Films
journal, June 2009

A theory of thin metal films: electron density, potentials and work function
journal, May 1976

Building Pb Nanomesas with Atomic-Layer Precision
journal, March 2004

Coverage-Dependent Collective Diffusion of a Dense Pb Wetting Layer on Si(111)
journal, January 2012

Coulomb Sink: A Novel Coulomb Effect on Coarsening of Metal Nanoclusters on Semiconductor Surfaces
journal, September 2004

Quantum size effect dependent critical size cluster and finite size effects
journal, May 2009

  • Binz, S. M.; Hupalo, M.; Tringides, M. C.
  • Journal of Applied Physics, Vol. 105, Issue 9
  • DOI: 10.1063/1.3121504

3D equilibrium crystal shapes in the new light of STM and AFM
journal, October 2003

Evidence for Quantum Size Effects Observed by Helium Atom Scattering during the Growth of Pb on Cu(111)
journal, October 1989

Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces
journal, April 2008

Correlations between In Situ Conductivity and Uniform-Height Epitaxial Morphology in Pb / Si ( 1 1 1 ) − ( 7 × 7 )
journal, February 2016

Thermal Stability and Electronic Structure of Atomically Uniform Pb Films on Si(111)
journal, July 2004

Soft self-consistent pseudopotentials in a generalized eigenvalue formalism
journal, April 1990

Morphological evolution during epitaxial thin film growth: Formation of 2D islands and 3D mounds
journal, April 2006

Theory of quantum size effects in thin Pb(111) films
journal, December 2002

Nature, Strength, and Consequences of Indirect Adsorbate Interactions on Metals
journal, August 2000

Quantum stabilities and growth modes of thin metal films: Unsupported and NiAl-supported Ag(110) and Ag(100)
journal, July 2008

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
  • DOI: 10.1063/1.1323224

Competition between area and height evolution of Pb islands on a Si(111) surface
journal, March 2009

Vacancy-Formation Energies in Metals from Positron Annihilation
journal, February 1972

Accelerated molecular dynamics simulation of thin-film growth with the bond-boost method
journal, January 2009

Kinetics of mesa overlayer growth: Climbing of adatoms onto the mesa top
journal, January 2008

  • Han, Yong; Liu, Feng; Li, Shao-Chun
  • Applied Physics Letters, Vol. 92, Issue 2
  • DOI: 10.1063/1.2827200

Controlling nucleation rates in nanostructures with electron confinement
journal, March 2010

Flat-surface, step-edge, facet–facet, and facet–step diffusion barriers in growth of a Pb mesa
journal, July 2008

Self-diffusion of adatoms on Ni(100) surfaces
journal, April 2001

Mechanisms of exchange diffusion on fcc(111) transition metal surfaces
journal, November 2005

    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Shapes of Fe nanocrystals encapsulated at the graphite surface
    journal, February 2020

      Sort by:
      [ × clear filter / sort ]

      Figures / Tables found in this record:

      TABLE I (p. 4)table
      FIG. 1 (p. 5)figure
      FIG. 2 (p. 6)figure
      TABLE II (p. 6)table
      FIG. 3 (p. 7)figure
      FIG. 4 (p. 8)figure
      FIG. 5 (p. 8)figure
      FIG. 6 (p. 9)figure
      FIG. 7 (p. 10)figure
      FIG. 8 (p. 10)figure
      FIG. 9 (p. 11)figure
      Figure-10 (p. 11)figure
      FIG. 11 (p. 12)figure
      FIG. 12 (p. 14)figure
      FIG. 13 (p. 14)figure
      TABLE III (p. 14)table
      FIG. 14 (p. 15)figure
        [ × clear filter / sort ]
        Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

        Similar Records in DOE PAGES and OSTI.GOV collections: