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Reshaping, Intermixing, and Coarsening for Metallic Nanocrystals: Nonequilibrium Statistical Mechanical and Coarse-Grained Modeling
Chemical Reviews
  • King C. Lai, Iowa State University and Ames Laboratory
  • Yong Han, Iowa State University and Ames Laboratory
  • Peter M. Spurgeon, Iowa State University
  • Wenyu Huang, Iowa State University
  • Patricia A. Thiel, Iowa State University and Ames Laboratory
  • Da-Jiang Liu, Ames Laboratory
  • James W. Evans, Iowa State University
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Submitted Manuscript
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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. 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.


This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Chemical Reviews, copyright © American Chemical Society after peer review. To access the final edited and published work see DOI: 10.1021/acs.chemrev.8b00582. Posted with permission.

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American Chemical Society
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King C. Lai, Yong Han, Peter M. Spurgeon, Wenyu Huang, et al.. "Reshaping, Intermixing, and Coarsening for Metallic Nanocrystals: Nonequilibrium Statistical Mechanical and Coarse-Grained Modeling" Chemical Reviews Vol. 119 Iss. 11 (2019) p. 6670 - 6768
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