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Transition state analysis of solid-solid transformations in nanocrystals

J. Chem. Phys. 131, 164116 (2009); doi:10.1063/1.3253700

Published 30 October 2009 | See: Publisher's Note

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Michael Grünwald1 and Christoph Dellago2
1Department of Chemistry, University of California at Berkeley, Berkeley, California 94720, USA
2Faculty of Physics and Center for Computational Materials Science, University of Vienna, Boltzmanngasse 5, 1090 Vienna, Austria
A systematic simulation methodology is introduced for the accurate determination of experimentally measurable quantities characterizing solid-solid phase transformations under pressure. The atomistic mechanisms of nucleation and growth in a structural transformation of pressurized CdSe nanocrystals are identified using transition path sampling computer simulation. A committor-based transition state analysis is applied to extract activation enthalpies and activation volumes from transformation pathways at experimental conditions. The qualitative dependence of activation enthalpies on nanocrystal size is in good agreement with experimental data and supports the observed nucleation mechanism, which is characterized by a critical nucleus of elongated shape located on the crystal surface. Based on committor distributions along typical transformation pathways, the coordination number is identified as a suitable reaction coordinate for the process. ©2009 American Institute of Physics
History: Received 24 March 2009; accepted 2 October 2009; published 30 October 2009; publisher error corrected 3 November 2009
Permalink: http://link.aip.org/link/?JCPSA6/131/164116/1
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ERRATUM

  1. Publisher's Note: “Transition state analysis of solid-solid transformations in nanocrystals” [J. Chem. Phys. 131, 164116 (2009)]
    Michael Grünwald et al.
    J. Chem. Phys. 131, 199901 (2009)

KEYWORDS and PACS

Keywords
PACS
  • 64.70.kg
    Solid-solid transitions in semiconductors
  • 61.46.Df
    Structure of nanocrystals and nanoparticles
  • 81.05.Dz
    II-VI semiconductors: fabrication, treatment, testing and analysis
  • 61.66.Fn
    Crystal structure of specific inorganic compounds
  • 65.80.+n
    Thermal properties of small particles, nanocrystals, nanotubes
  • YEAR: 2009

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PUBLICATION DATA

ISSN:
0021-9606 (print)   1089-7690 (online)
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