Reshaping, Intermixing, and Coarsening for Metallic Nanocrystals: Nonequilibrium Statistical Mechanical and Coarse-Grained Modeling

Lai, King C.; Han, Yong; Spurgeon, Peter; Huang, Wenyu; Thiel, Patricia A.; Liu, Da-Jiang; Evans, James W.

doi:10.1021/acs.chemrev.8b00582

Reshaping, Intermixing, and Coarsening for Metallic Nanocrystals: Nonequilibrium Statistical Mechanical and Coarse-Grained Modeling

Journal Article · Tue Jun 04 00:00:00 EDT 2019 · Chemical Reviews

DOI:https://doi.org/10.1021/acs.chemrev.8b00582· OSTI ID:1542947

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

Self-assembly of supported 2D or 3D nanocrystals (NCs) by vacuum deposition and of 3D NCs by solution-phase synthesis (with possible subsequent transfer to a support) produces intrinsically nonequilibrium systems. Individual NCs can have far-from-equilibrium shapes and composition profiles. The free energy of NC ensembles is lowered by coarsening which can involve Ostwald ripening or Smoluchowski ripening (NC diffusion and coalescence). Preservation of individual NC structure and inhibition of coarsening are key, e.g., for avoiding catalyst degradation. This review focuses on postsynthesis evolution of metallic NCs. Atomistic-level modeling typically utilizes stochastic lattice-gas models to access appropriate time and length scales. However, predictive modeling requires incorporation of realistic rates for relaxation mechanisms, e.g., periphery diffusion and intermixing, in numerous local environments (rather than the use of generic prescriptions). Alternative coarse-grained modeling must also incorporate appropriate mechanisms and kinetics. At the level of individual NCs, we present analyses of reshaping, including sintering and pinch-off, and of compositional evolution in a vacuum environment. Here, we also discuss modeling of coarsening including diffusion and decay of individual NCs and unconventional coarsening processes. We describe high-level modeling integrated with scanning tunneling microscopy (STM) studies for supported 2D epitaxial nanoclusters and developments in modeling for 3D NCs motivated by in situ transmission electron microscopy (TEM) studies.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1542947

Report Number(s):: IS-J--9764

Journal Information:: Chemical Reviews, Journal Name: Chemical Reviews Journal Issue: 11 Vol. 119; ISSN 0009-2665

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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