DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Direct observations of shape fluctuation in long-time atomistic simulations of metallic nanoclusters

Abstract

Metallic nanoclusters are functional materials whose unique physical and chemical properties are sensitively controlled by their shapes and structures. An in-depth understanding of their morphological stability is therefore of crucial importance. It has been well documented by transmission electron microscopy (TEM) studies that metallic nanoclusters can interconvert between different isomers. However, the relevant mechanisms remain elusive because the timescales of such shape fluctuations are too short to be resolved experimentally and yet too long for conventional atomistic simulations. By employing massively parallel accelerated molecular dynamics (AMD) simulations reaching timescales of milliseconds, here we provide a clear description of the dynamical processes leading to shape fluctuation in metallic nanoclusters of platinum, silver, copper, and gold at different sizes and temperatures. In all these materials, direct transformations between face-centered-cubic and fivefold symmetric structures (decahedron or icosahedron) are observed away from the melting point. These transitions occur following either a slip-mediated twinning mechanism or a surface-reconstruction driven process. The identified pathways are shown to be reversible, allowing for genuine shape fluctuation processes that do not involve melting or other external factors.

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [3]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Xiamen Univ. (China)
  2. Xiamen Univ. (China)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1688775
Alternate Identifier(s):
OSTI ID: 1488885
Report Number(s):
LA-UR-17-22655
Journal ID: ISSN 2475-9953 (Electronic); TRN: US2204248
Grant/Contract Number:  
89233218CNA000001; AC52-06NA25396; 51871189; 11474234; 20150557ER
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 12; Journal ID: ISSN 2475-9953 (Electronic)
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Material Science

Citation Formats

Huang, Rao, Wen, Yuhua, Voter, Arthur Ford, and Perez, Danny. Direct observations of shape fluctuation in long-time atomistic simulations of metallic nanoclusters. United States: N. p., 2018. Web. doi:10.1103/PhysRevMaterials.2.126002.
Huang, Rao, Wen, Yuhua, Voter, Arthur Ford, & Perez, Danny. Direct observations of shape fluctuation in long-time atomistic simulations of metallic nanoclusters. United States. https://doi.org/10.1103/PhysRevMaterials.2.126002
Huang, Rao, Wen, Yuhua, Voter, Arthur Ford, and Perez, Danny. Wed . "Direct observations of shape fluctuation in long-time atomistic simulations of metallic nanoclusters". United States. https://doi.org/10.1103/PhysRevMaterials.2.126002. https://www.osti.gov/servlets/purl/1688775.
@article{osti_1688775,
title = {Direct observations of shape fluctuation in long-time atomistic simulations of metallic nanoclusters},
author = {Huang, Rao and Wen, Yuhua and Voter, Arthur Ford and Perez, Danny},
abstractNote = {Metallic nanoclusters are functional materials whose unique physical and chemical properties are sensitively controlled by their shapes and structures. An in-depth understanding of their morphological stability is therefore of crucial importance. It has been well documented by transmission electron microscopy (TEM) studies that metallic nanoclusters can interconvert between different isomers. However, the relevant mechanisms remain elusive because the timescales of such shape fluctuations are too short to be resolved experimentally and yet too long for conventional atomistic simulations. By employing massively parallel accelerated molecular dynamics (AMD) simulations reaching timescales of milliseconds, here we provide a clear description of the dynamical processes leading to shape fluctuation in metallic nanoclusters of platinum, silver, copper, and gold at different sizes and temperatures. In all these materials, direct transformations between face-centered-cubic and fivefold symmetric structures (decahedron or icosahedron) are observed away from the melting point. These transitions occur following either a slip-mediated twinning mechanism or a surface-reconstruction driven process. The identified pathways are shown to be reversible, allowing for genuine shape fluctuation processes that do not involve melting or other external factors.},
doi = {10.1103/PhysRevMaterials.2.126002},
journal = {Physical Review Materials},
number = 12,
volume = 2,
place = {United States},
year = {Wed Dec 26 00:00:00 EST 2018},
month = {Wed Dec 26 00:00:00 EST 2018}
}

Journal Article:

Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Structural Dynamics of Low-Symmetry Au Nanoparticles Stimulated by Electron Irradiation
journal, October 2011

  • Zhang, Bingsen; Wang, Di; Zhang, Wei
  • Chemistry - A European Journal, Vol. 17, Issue 46
  • DOI: 10.1002/chem.201102092

Size-Dependent Catalytic Activity and Dynamics of Gold Nanoparticles at the Single-Molecule Level
journal, January 2010

  • Zhou, Xiaochun; Xu, Weilin; Liu, Guokun
  • Journal of the American Chemical Society, Vol. 132, Issue 1
  • DOI: 10.1021/ja904307n

Structural fluctuations in small particles
journal, April 1988


Morphology transition mechanism from icosahedral to decahedral phase during growth of Cu nanoclusters
journal, July 2015


Accurate Interatomic Potentials for Ni, Al and Ni3Al
journal, January 1986


On fitting a gold embedded atom method potential using the force matching method
journal, November 2005

  • Grochola, Gregory; Russo, Salvy P.; Snook, Ian K.
  • The Journal of Chemical Physics, Vol. 123, Issue 20
  • DOI: 10.1063/1.2124667

Time-Dependent Density Functional Theory Studies of Optical Properties of Au Nanoparticles: Octahedra, Truncated Octahedra, and Icosahedra
journal, September 2015

  • Bae, Gyun-Tack; Aikens, Christine M.
  • The Journal of Physical Chemistry C, Vol. 119, Issue 40
  • DOI: 10.1021/acs.jpcc.5b05978

An embedded-atom potential for the Cu–Ag system
journal, May 2006

  • Williams, P. L.; Mishin, Y.; Hamilton, J. C.
  • Modelling and Simulation in Materials Science and Engineering, Vol. 14, Issue 5
  • DOI: 10.1088/0965-0393/14/5/002

Long-time molecular dynamics simulations on massively parallel platforms: A comparison of parallel replica dynamics and parallel trajectory splicing
journal, December 2017

  • Perez, Danny; Huang, Rao; Voter, Arthur F.
  • Journal of Materials Research, Vol. 33, Issue 7
  • DOI: 10.1557/jmr.2017.456

Electron microscopy: Coulomb explosions in metals?
journal, April 1986


A mathematical formalization of the parallel replica dynamics
journal, January 2012

  • Le Bris, Claude; Lelièvre, Tony; Luskin, Mitchell
  • Monte Carlo Methods and Applications, Vol. 18, Issue 2
  • DOI: 10.1515/mcma-2012-0003

Robust Perron cluster analysis in conformation dynamics
journal, March 2005


Structural changes accompanying densification of random hard-sphere packings
journal, June 1993


Automated identification and indexing of dislocations in crystal interfaces
journal, October 2012

  • Stukowski, Alexander; Bulatov, Vasily V.; Arsenlis, Athanasios
  • Modelling and Simulation in Materials Science and Engineering, Vol. 20, Issue 8
  • DOI: 10.1088/0965-0393/20/8/085007

Stepwise Evolution of Spherical Seeds into 20-Fold Twinned Icosahedra
journal, August 2012


Dynamic Atomic-Level Rearrangements in Small Gold Particles
journal, August 1986


Long-Time Dynamics through Parallel Trajectory Splicing
journal, December 2015

  • Perez, Danny; Cubuk, Ekin D.; Waterland, Amos
  • Journal of Chemical Theory and Computation, Vol. 12, Issue 1
  • DOI: 10.1021/acs.jctc.5b00916

Time-resolved electron microscopy studies of the structure of nanoparticles and their melting
journal, November 2001


Structural fluctuation of Au55 and Au147 clusters: Substrate effect
journal, December 1992

  • Sawada, S.; Sugano, S.
  • Zeitschrift f�r Physik D Atoms, Molecules and Clusters, Vol. 24, Issue 4
  • DOI: 10.1007/BF01426687

Structure, thermodynamics, and rearrangement mechanisms in gold clusters—insights from the energy landscapes framework
journal, January 2018

  • Schebarchov, D.; Baletto, F.; Wales, D. J.
  • Nanoscale, Vol. 10, Issue 4
  • DOI: 10.1039/C7NR07123J

Melting of Gold Clusters: Icosahedral Precursors
journal, September 1998


The parallel replica dynamics method – Coming of age
journal, April 2015


Revisiting the structural instability observed in small particles in the electron microscope
journal, June 1993

  • Ugarte, Daniel
  • Zeitschrift f�r Physik D Atoms, Molecules and Clusters, Vol. 28, Issue 2
  • DOI: 10.1007/BF01436986

Changes of Morphology and Capping of Model Transition Metal Clusters
journal, January 1996

  • Wales, David J.; Munro, Lindsey J.
  • The Journal of Physical Chemistry, Vol. 100, Issue 6
  • DOI: 10.1021/jp952521s

Metallic nanoparticles meet metadynamics
journal, November 2015

  • Pavan, L.; Rossi, K.; Baletto, F.
  • The Journal of Chemical Physics, Vol. 143, Issue 18
  • DOI: 10.1063/1.4935272

Structural stability and lattice defects in copper: Ab initio , tight-binding, and embedded-atom calculations
journal, May 2001


Metastability of the atomic structures of size-selected gold nanoparticles
journal, January 2015

  • Wells, Dawn M.; Rossi, Giulia; Ferrando, Riccardo
  • Nanoscale, Vol. 7, Issue 15
  • DOI: 10.1039/C4NR05811A

Microscopic mechanisms of the growth of metastable silver icosahedra
journal, March 2001


Cluster analysis of accelerated molecular dynamics simulations: A case study of the decahedron to icosahedron transition in Pt nanoparticles
journal, October 2017

  • Huang, Rao; Lo, Li-Ta; Wen, Yuhua
  • The Journal of Chemical Physics, Vol. 147, Issue 15
  • DOI: 10.1063/1.4996922

Shape- and Symmetry-Dependent Mechanical Properties of Metallic Gold and Silver on the Nanoscale
journal, January 2014

  • Mahmoud, Mahmoud A.; O’Neil, Daniel; El-Sayed, Mostafa A.
  • Nano Letters, Vol. 14, Issue 2
  • DOI: 10.1021/nl4040362

Single-molecule nanocatalysis reveals heterogeneous reaction pathways and catalytic dynamics
journal, November 2008

  • Xu, Weilin; Kong, Jason S.; Yeh, Yun-Ting E.
  • Nature Materials, Vol. 7, Issue 12
  • DOI: 10.1038/nmat2319

Transition from Icosahedral to Decahedral Structure in a Coexisting Solid-Liquid Nickel Cluster
journal, September 2005


Melting and Freezing Characteristics and Structural Properties of Supported and Unsupported Gold Nanoclusters
journal, July 2005

  • Kuo, Chin-Lung; Clancy, Paulette
  • The Journal of Physical Chemistry B, Vol. 109, Issue 28
  • DOI: 10.1021/jp0518862

Size-dependent crystalline fluctuation and growth mechanism of bismuth nanoparticles under electron beam irradiation
journal, January 2016


Observation time scale, free-energy landscapes, and molecular symmetry
journal, December 2013

  • Wales, D. J.; Salamon, P.
  • Proceedings of the National Academy of Sciences, Vol. 111, Issue 2
  • DOI: 10.1073/pnas.1319599111

Experimental studies of small particle structures
journal, June 1994


Motion of small gold clusters in the electron microscope
journal, June 1987

  • Williams, Peter
  • Applied Physics Letters, Vol. 50, Issue 24
  • DOI: 10.1063/1.97739

Solid-liquid phase coexistence and structural transitions in palladium clusters
journal, March 2006


Structural stability of icosahedral FePt nanoparticles
journal, January 2009

  • Wang, Rongming; Zhang, Hongzhou; Farle, Michael
  • Nanoscale, Vol. 1, Issue 2
  • DOI: 10.1039/b9nr00096h