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Title: Entropic description of gas hydrate ice/liquid equilibrium via enhanced sampling of coexisting phases

Abstract

Metastable β ice holds small guest molecules in stable gas hydrates, so its solid/liquid equilibrium is of interest. However, aqueous crystal/liquid transitions are very difficult to simulate. A new MD algorithm generates trajectories in a generalized NPT ensemble and equilibrates states of coexisting phases with a selectable enthalpy. Furthermore, with replicas spanning the range between β ice and liquid water we find the statistical temperature from the enthalpy histograms and characterize the transition by the entropy, introducing a general computational procedure for first-order transitions.

Authors:
 [1];  [2];  [1]
+ Show Author Affiliations
  1. Boston Univ., Boston, MA (United States)
  2. Broad Institute of Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Harvard Univ., Cambridge, MA (United States)
Publication Date:
Research Org.:
Boston Univ., MA (United States)
Sponsoring Org.:
USDOE
Contributing Org.:
Boston University Center for Computational Science
OSTI Identifier:
1247480
Alternate Identifier(s):
OSTI ID: 1181418
Grant/Contract Number:  
SC0008810
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 114; Journal Issue: 17; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 97 MATHEMATICS AND COMPUTING; hydrates; phase transitions; computer simulation; algorithm design

Citation Formats

Malolepsza, Edyta, Kim, Jaegil, and Keyes, Tom. Entropic description of gas hydrate ice/liquid equilibrium via enhanced sampling of coexisting phases. United States: N. p., 2015. Web. doi:10.1103/PhysRevLett.114.170601.
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Malolepsza, Edyta, Kim, Jaegil, & Keyes, Tom. Entropic description of gas hydrate ice/liquid equilibrium via enhanced sampling of coexisting phases. United States. https://doi.org/10.1103/PhysRevLett.114.170601
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Malolepsza, Edyta, Kim, Jaegil, and Keyes, Tom. Tue . "Entropic description of gas hydrate ice/liquid equilibrium via enhanced sampling of coexisting phases". United States. https://doi.org/10.1103/PhysRevLett.114.170601. https://www.osti.gov/servlets/purl/1247480.
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@article{osti_1247480,
title = {Entropic description of gas hydrate ice/liquid equilibrium via enhanced sampling of coexisting phases},
author = {Malolepsza, Edyta and Kim, Jaegil and Keyes, Tom},
abstractNote = {Metastable β ice holds small guest molecules in stable gas hydrates, so its solid/liquid equilibrium is of interest. However, aqueous crystal/liquid transitions are very difficult to simulate. A new MD algorithm generates trajectories in a generalized NPT ensemble and equilibrates states of coexisting phases with a selectable enthalpy. Furthermore, with replicas spanning the range between β ice and liquid water we find the statistical temperature from the enthalpy histograms and characterize the transition by the entropy, introducing a general computational procedure for first-order transitions.},
doi = {10.1103/PhysRevLett.114.170601},
journal = {Physical Review Letters},
number = 17,
volume = 114,
place = {United States},
year = {Tue Apr 28 00:00:00 EDT 2015},
month = {Tue Apr 28 00:00:00 EDT 2015}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1103/PhysRevLett.114.170601
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