Communication: Diverse nanoscale cluster dynamics: Diffusion of 2D epitaxial clusters

Lai, King C.; Evans, James W.; Liu, Da -Jiang

doi:10.1063/1.5008424

Title: Communication: Diverse nanoscale cluster dynamics: Diffusion of 2D epitaxial clusters

Abstract

The dynamics of nanoscale clusters can be distinct from macroscale behavior described by continuum formalisms. For diffusion of 2D clusters of N atoms in homoepitaxial systems mediated by edge atom hopping, macroscale theory predicts simple monotonic size scaling of the diffusion coefficient, D_N ~ N^–β, with β = 3/2. However, modeling for nanoclusters on metal(100) surfaces reveals that slow nucleation-mediated diffusion displaying weak size scaling β < 1 occurs for “perfect” sizes N_p = L² and L(L+1) for integer L = 3,4,… (with unique square or near-square ground state shapes), and also for N_p+3, N_p+4,…. In contrast, fast facile nucleation-free diffusion displaying strong size scaling β ≈ 2.5 occurs for sizes N_p+1 and N_p+2. D_N versus N oscillates strongly between the slowest branch (for N_p+3) and the fastest branch (for N_p+1). All branches merge for N = O(10²), but macroscale behavior is only achieved for much larger N = O(10³). Here, this analysis reveals the unprecedented diversity of behavior on the nanoscale.

Authors:

Lai, King C. ^[1];

^[1];

^[1]

Ames Lab. and Iowa State Univ., Ames, IA (United States)

Publication Date:: Mon Nov 27 00:00:00 EST 2017

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

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

OSTI Identifier:: 1411951

Alternate Identifier(s):: OSTI ID: 1410400

Report Number(s):: IS-J-9460
Journal ID: ISSN 0021-9606; TRN: US1800287

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

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 147; Journal Issue: 20; Journal ID: ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Lai, King C., Evans, James W., and Liu, Da -Jiang. Communication: Diverse nanoscale cluster dynamics: Diffusion of 2D epitaxial clusters.  United States: N. p., 2017. 
Web.  doi:10.1063/1.5008424.

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                    Lai, King C., Evans, James W., & Liu, Da -Jiang. Communication: Diverse nanoscale cluster dynamics: Diffusion of 2D epitaxial clusters.  United States.  https://doi.org/10.1063/1.5008424

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                    Lai, King C., Evans, James W., and Liu, Da -Jiang. Mon .  
"Communication: Diverse nanoscale cluster dynamics: Diffusion of 2D epitaxial clusters".  United States.  https://doi.org/10.1063/1.5008424.  https://www.osti.gov/servlets/purl/1411951.

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@article{osti_1411951,

  title        = {Communication: Diverse nanoscale cluster dynamics: Diffusion of 2D epitaxial clusters},

  author       = {Lai, King C. and Evans, James W. and Liu, Da -Jiang},

  abstractNote = {The dynamics of nanoscale clusters can be distinct from macroscale behavior described by continuum formalisms. For diffusion of 2D clusters of N atoms in homoepitaxial systems mediated by edge atom hopping, macroscale theory predicts simple monotonic size scaling of the diffusion coefficient, DN ~ N–β, with β = 3/2. However, modeling for nanoclusters on metal(100) surfaces reveals that slow nucleation-mediated diffusion displaying weak size scaling β < 1 occurs for “perfect” sizes Np = L2 and L(L+1) for integer L = 3,4,… (with unique square or near-square ground state shapes), and also for Np+3, Np+4,…. In contrast, fast facile nucleation-free diffusion displaying strong size scaling β ≈ 2.5 occurs for sizes Np+1 and Np+2. DN versus N oscillates strongly between the slowest branch (for Np+3) and the fastest branch (for Np+1). All branches merge for N = O(102), but macroscale behavior is only achieved for much larger N = O(103). Here, this analysis reveals the unprecedented diversity of behavior on the nanoscale.},

  doi          = {10.1063/1.5008424},

  journal      = {Journal of Chemical Physics},

  number       = 20,

  volume       = 147,

  place        = {United States},

  year         = {Mon Nov 27 00:00:00 EST 2017},

  month        = {Mon Nov 27 00:00:00 EST 2017}

}

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Works referencing / citing this record:

Complex oscillatory decrease with size in diffusivity of {100}-epitaxially supported 3D fcc metal nanoclusters
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Title: Communication: Diverse nanoscale cluster dynamics: Diffusion of 2D epitaxial clusters

Abstract

Citation Formats

Nucleation Barrier for Volume-Conserving Shape Changes of Faceted Crystals journal, January 2000

Relaxation kinetics in two-dimensional structures journal, November 2003

Fundamental Insight into the Substrate-Dependent Ripening of Monodisperse Clusters journal, August 2013

Formation, Stability, and Breakup of Nanojets journal, August 2000

Ehrlich-Schwoebel barrier and interface-limited decay in island kinetics on Ag(100) journal, January 2012

Real-Time TEM and Kinetic Monte Carlo Studies of the Coalescence of Decahedral Gold Nanoparticles journal, October 2009

Simulations of mobility and evaporation rate of adsorbate islands on solid surfaces journal, November 1999

Evolution of Two-Dimensional Wormlike Nanoclusters on Metal Surfaces journal, April 2001

Island Diffusion on Metal fcc (100) Surfaces journal, March 1999

Some aspects of cluster diffusion on surfaces journal, July 1982

Island Diffusion and Coarsening on Metal (100) Surfaces journal, October 1997

Coarsening of Two-Dimensional Nanoclusters on Metal Surfaces journal, March 2009

CO-Induced Smoluchowski Ripening of Pt Cluster Arrays on the Graphene/Ir(111) Moiré journal, February 2013

Diffusion of small clusters on metal (100) surfaces: Exact master-equation analysis for lattice-gas models journal, January 1999

Thin-film cliffhanger journal, June 2002

Modeling the Migration of Platinum Nanoparticles on Surfaces Using a Kinetic Monte Carlo Approach journal, February 2017

Kinetics of shape equilibration for two dimensional islands journal, October 1999

Continuum Model for Low Temperature Relaxation of Crystal Steps journal, August 2001

Sintering of Catalytic Nanoparticles: Particle Migration or Ostwald Ripening? journal, April 2013

Sintering of two-dimensional nanoclusters in metal(100) homoepitaxial systems: Deviations from predictions of Mullins continuum theory journal, October 2002

Nonequilibrium kinetic study of sintering of dispersed nanoparticles journal, January 2013

Evolution of Far-From-Equilibrium Nanostructures Formed by Cluster-Step and Cluster-Cluster Coalescence in Metal Films journal, October 1998

Random Walks on Lattices. II journal, February 1965

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

Step-Energy Barriers and Particle Shape Changes during Coarsening journal, March 2002

QM/MD studies on graphene growth from small islands on the Ni(111) surface journal, January 2016

Fast scanning tunnelling microscopy as a tool to understand changes on metal surfaces: from nanostructures to single atoms journal, March 2005

Adatom mobility for the solid-on-solid model journal, June 1995

Evolution of neck radius and relaxation of coalescing nanoparticles journal, August 2009

Continuum Model for Low Temperature Relaxation of Crystal Steps text, January 2001

Nonequilibrium Kinetic Study of Sintering of Dispersed Nanoparticles text, January 2013

Relaxation kinetics in two-dimensional structures text, January 2003

Kinetics of shape equilibration for two-dimensional islands text, January 1999

Island diffusion on metal fcc(100) surfaces text, January 1999

Complex oscillatory decrease with size in diffusivity of {100}-epitaxially supported 3D fcc metal nanoclusters journal, January 2019

Nucleation Barrier for Volume-Conserving Shape Changes of Faceted Crystals
journal, January 2000

Relaxation kinetics in two-dimensional structures
journal, November 2003

Fundamental Insight into the Substrate-Dependent Ripening of Monodisperse Clusters
journal, August 2013

Formation, Stability, and Breakup of Nanojets
journal, August 2000

Ehrlich-Schwoebel barrier and interface-limited decay in island kinetics on Ag(100)
journal, January 2012

Real-Time TEM and Kinetic Monte Carlo Studies of the Coalescence of Decahedral Gold Nanoparticles
journal, October 2009

Simulations of mobility and evaporation rate of adsorbate islands on solid surfaces
journal, November 1999

Evolution of Two-Dimensional Wormlike Nanoclusters on Metal Surfaces
journal, April 2001

Island Diffusion on Metal fcc (100) Surfaces
journal, March 1999

Some aspects of cluster diffusion on surfaces
journal, July 1982

Island Diffusion and Coarsening on Metal (100) Surfaces
journal, October 1997

Coarsening of Two-Dimensional Nanoclusters on Metal Surfaces
journal, March 2009

CO-Induced Smoluchowski Ripening of Pt Cluster Arrays on the Graphene/Ir(111) Moiré
journal, February 2013

Diffusion of small clusters on metal (100) surfaces: Exact master-equation analysis for lattice-gas models
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journal, June 2002

Modeling the Migration of Platinum Nanoparticles on Surfaces Using a Kinetic Monte Carlo Approach
journal, February 2017

Kinetics of shape equilibration for two dimensional islands
journal, October 1999

Continuum Model for Low Temperature Relaxation of Crystal Steps
journal, August 2001

Sintering of Catalytic Nanoparticles: Particle Migration or Ostwald Ripening?
journal, April 2013

Sintering of two-dimensional nanoclusters in metal(100) homoepitaxial systems: Deviations from predictions of Mullins continuum theory
journal, October 2002

Nonequilibrium kinetic study of sintering of dispersed nanoparticles
journal, January 2013

Evolution of Far-From-Equilibrium Nanostructures Formed by Cluster-Step and Cluster-Cluster Coalescence in Metal Films
journal, October 1998

Random Walks on Lattices. II
journal, February 1965

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

Step-Energy Barriers and Particle Shape Changes during Coarsening
journal, March 2002

QM/MD studies on graphene growth from small islands on the Ni(111) surface
journal, January 2016

Fast scanning tunnelling microscopy as a tool to understand changes on metal surfaces: from nanostructures to single atoms
journal, March 2005

Adatom mobility for the solid-on-solid model
journal, June 1995

Evolution of neck radius and relaxation of coalescing nanoparticles
journal, August 2009

Continuum Model for Low Temperature Relaxation of Crystal Steps
text, January 2001

Nonequilibrium Kinetic Study of Sintering of Dispersed Nanoparticles
text, January 2013

Relaxation kinetics in two-dimensional structures
text, January 2003

Kinetics of shape equilibration for two-dimensional islands
text, January 1999

Island diffusion on metal fcc(100) surfaces
text, January 1999

Complex oscillatory decrease with size in diffusivity of {100}-epitaxially supported 3D fcc metal nanoclusters
journal, January 2019