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Title: Many-Body Interactions in Ice

Many-body effects in ice are investigated through a systematic analysis of the lattice energies of several proton ordered and disordered phases, which are calculated with different flexible water models, ranging from pairwise additive (q-TIP4P/F) to polarizable (TTM3-F and AMOE-BA BA) and explicit many-body (MB-pol) potential energy functions. Comparisons with available experimental and diffusion Monte Carlo data emphasize the importance of an accurate description of the individual terms of the many-body expansion of the interaction energy between water molecules for the correct prediction of the energy ordering of the ice phases. Further analysis of the MB-pol results, in terms of fundamental energy contributions, demonstrates that the differences in lattice energies between different ice phases are sensitively dependent on the subtle balance between short-range two-body and three-body interactions, many-body induction, and dispersion energy. Here, by correctly reproducing many-body effects at both short range and long range, it is found that MB-pol accurately predicts the energetics of different ice phases, which provides further support for the accuracy of MB-pol in representing the properties of water from the gas to the condensed phase.
Authors:
 [1] ;  [1] ;  [1] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Univ. of California - San Diego, La Jolla, CA (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Theory and Computation
Additional Journal Information:
Journal Volume: 13; Journal Issue: 4; Journal ID: ISSN 1549-9618
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
National Science Foundation (NSF); Argonne National Laboratory, Argonne Leadership Computing Facility
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1373735

Pham, C. Huy, Reddy, Sandeep K., Chen, Karl, Knight, Chris, and Paesani, Francesco. Many-Body Interactions in Ice. United States: N. p., Web. doi:10.1021/acs.jctc.6b01248.
Pham, C. Huy, Reddy, Sandeep K., Chen, Karl, Knight, Chris, & Paesani, Francesco. Many-Body Interactions in Ice. United States. doi:10.1021/acs.jctc.6b01248.
Pham, C. Huy, Reddy, Sandeep K., Chen, Karl, Knight, Chris, and Paesani, Francesco. 2017. "Many-Body Interactions in Ice". United States. doi:10.1021/acs.jctc.6b01248. https://www.osti.gov/servlets/purl/1373735.
@article{osti_1373735,
title = {Many-Body Interactions in Ice},
author = {Pham, C. Huy and Reddy, Sandeep K. and Chen, Karl and Knight, Chris and Paesani, Francesco},
abstractNote = {Many-body effects in ice are investigated through a systematic analysis of the lattice energies of several proton ordered and disordered phases, which are calculated with different flexible water models, ranging from pairwise additive (q-TIP4P/F) to polarizable (TTM3-F and AMOE-BA BA) and explicit many-body (MB-pol) potential energy functions. Comparisons with available experimental and diffusion Monte Carlo data emphasize the importance of an accurate description of the individual terms of the many-body expansion of the interaction energy between water molecules for the correct prediction of the energy ordering of the ice phases. Further analysis of the MB-pol results, in terms of fundamental energy contributions, demonstrates that the differences in lattice energies between different ice phases are sensitively dependent on the subtle balance between short-range two-body and three-body interactions, many-body induction, and dispersion energy. Here, by correctly reproducing many-body effects at both short range and long range, it is found that MB-pol accurately predicts the energetics of different ice phases, which provides further support for the accuracy of MB-pol in representing the properties of water from the gas to the condensed phase.},
doi = {10.1021/acs.jctc.6b01248},
journal = {Journal of Chemical Theory and Computation},
number = 4,
volume = 13,
place = {United States},
year = {2017},
month = {2}
}