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

Journal Article · · Physical Review B
 [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
+ Show Author Affiliations

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).

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC02-07CH11358
OSTI ID:
1544356
Alternate ID(s):
OSTI ID: 1407439
Journal Information:
Physical Review B, Vol. 96, Issue 20; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 13 works
Citation information provided by
Web of Science

References (74)

Fabricating artificial nanowells with tunable size and shape by using scanning tunneling microscopy journal September 2006
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
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
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
Diffusion of Cu on Cu surfaces journal August 1995
Observation of preferred heights in Pb nanoislands: A quantum size effect journal September 2002
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
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
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
Quantum size effects on the work function of metallic thin film nanostructures journal July 2010
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
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
Use of Thermal Expansion Measurements to Detect Lattice Vacancies near the Melting Point of Pure Lead and Aluminum journal March 1958
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
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
Controlling nucleation rates in nanostructures with electron confinement journal March 2010
Quantum size effects in metal nanofilms: Comparison of an electron-gas model and density functional theory calculations journal October 2009
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

Cited By (1)

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

Figures / Tables (17)

TABLE I(p. 4)table TABLE I
FIG. 1(p. 5)figure FIG. 1
FIG. 2(p. 6)figure FIG. 2
TABLE II(p. 6)table TABLE II
FIG. 3(p. 7)figure FIG. 3
FIG. 4(p. 8)figure FIG. 4
FIG. 5(p. 8)figure FIG. 5
FIG. 6(p. 9)figure FIG. 6
FIG. 7(p. 10)figure FIG. 7
FIG. 8(p. 10)figure FIG. 8
FIG. 9(p. 11)figure FIG. 9
Figure-10(p. 11)figure Figure-10
FIG. 11(p. 12)figure FIG. 11
FIG. 12(p. 14)figure FIG. 12
FIG. 13(p. 14)figure FIG. 13
TABLE III(p. 14)table TABLE III
FIG. 14(p. 15)figure FIG. 14

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