Papers

Peer-reviewed
Aug 21, 2011

Order parameters for the multistep crystallization of clathrate hydrates

Journal of Chemical Physics
  • Liam C. Jacobson
  • ,
  • Masakazu Matsumoto
  • ,
  • Valeria Molinero

Volume
135
Number
7
Language
English
Publishing type
Research paper (scientific journal)
DOI
10.1063/1.3613667

Recent reports indicate that the crystallization of clathrate hydrates occurs in multiple steps that involve amorphous intermediates and metastable clathrate crystals. The elucidation of the reaction coordinate for clathrate crystallization requires the use of order parameters able to identify the reactants, products, and intermediates in the crystallization pathway. Nevertheless, existing order parameters cannot distinguish between amorphous and crystalline clathrates or between different clathrate crystals. In this work, we present the first set of order parameters that discern between the sI and sII clathrate crystals, the amorphous clathrates, the blob of solvent-separated guests and the liquid solution. These order parameters can be used to monitor the advance of the crystallization and for the efficient implementation of methods to sample the rare clathrate nucleation events in molecular simulations. We illustrate the use of these order parameters in the analysis of the growth and the dissolution of clathrate crystals and the spontaneous nucleation and growth of clathrates under conditions of high supercooling. © 2011 American Institute of Physics.

Link information
DOI
https://doi.org/10.1063/1.3613667
URL
http://www.scopus.com/inward/record.url?eid=2-s2.0-80052050460&partnerID=MN8TOARS
ID information
  • DOI : 10.1063/1.3613667
  • ISSN : 0021-9606
  • ORCID - Put Code : 25798642
  • SCOPUS ID : 80052050460

Export
BibTeX RIS