skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Exploring the Rich Potential Energy Surface of (H 2O) 11 and Its Physical Implications

Abstract

The rich potential energy surface of the water undecamer (H 2O) 11 was explored with a basin hopping algorithm using a TIP 4P potential and other methods followed by extensive ab initio MP2 minimizations and CCSD(T) corrections. This protocol yielded 17, 66, and 125 distinct isomers within 0.5, 1.0, and 2.0 kcal mol –1 of the complete basis set CCSD(T) global minimum, respectively. These isomers were categorized into 15 different families based on their oxygen framework and hydrogen bonding topology. Determination of the global minimum proved challenging because of the presence of many nearly isoenergetic isomers. The predicted global minimum varied among ab initio methods, density functionals, and model potentials, and it was sensitive to the choice of energy extrapolation schemes, higher-order CCSD(T) corrections, and inclusion of zero-point vibrational energy. In conclusion, the presence of a large number of nearly degenerate structures and the isomerization between them has manifested itself in the anomalous broadening of the heat capacity curve of the undecamer in simulations around the melting region.

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [3];  [4];  [5]; ORCiD logo [1]
  1. Furman Univ., Greenville, SC (United States); Bucknell Univ., Lewisburg, PA (United States)
  2. Bucknell Univ., Lewisburg, PA (United States)
  3. Univ. of Virginia, Charlottesville, VA (United States); Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany)
  4. Univ. of Virginia, Charlottesville, VA (United States)
  5. Polish Academy of Sciences, Warszawa (Poland)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1480244
Grant/Contract Number:  
AC02-05CH11231; CHE-1213521; CHE-1508556; CHE-1229354; TG-CHE120025
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Theory and Computation
Additional Journal Information:
Journal Volume: 14; Journal Issue: 2; Journal ID: ISSN 1549-9618
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Temelso, Berhane, Klein, Katurah L., Mabey, Joel W., Pérez, Cristóbal, Pate, Brooks H., Kisiel, Zbigniew, and Shields, George C. Exploring the Rich Potential Energy Surface of (H2O)11 and Its Physical Implications. United States: N. p., 2018. Web. doi:10.1021/acs.jctc.7b00938.
Temelso, Berhane, Klein, Katurah L., Mabey, Joel W., Pérez, Cristóbal, Pate, Brooks H., Kisiel, Zbigniew, & Shields, George C. Exploring the Rich Potential Energy Surface of (H2O)11 and Its Physical Implications. United States. doi:10.1021/acs.jctc.7b00938.
Temelso, Berhane, Klein, Katurah L., Mabey, Joel W., Pérez, Cristóbal, Pate, Brooks H., Kisiel, Zbigniew, and Shields, George C. Fri . "Exploring the Rich Potential Energy Surface of (H2O)11 and Its Physical Implications". United States. doi:10.1021/acs.jctc.7b00938. https://www.osti.gov/servlets/purl/1480244.
@article{osti_1480244,
title = {Exploring the Rich Potential Energy Surface of (H2O)11 and Its Physical Implications},
author = {Temelso, Berhane and Klein, Katurah L. and Mabey, Joel W. and Pérez, Cristóbal and Pate, Brooks H. and Kisiel, Zbigniew and Shields, George C.},
abstractNote = {The rich potential energy surface of the water undecamer (H2O)11 was explored with a basin hopping algorithm using a TIP4P potential and other methods followed by extensive ab initio MP2 minimizations and CCSD(T) corrections. This protocol yielded 17, 66, and 125 distinct isomers within 0.5, 1.0, and 2.0 kcal mol–1 of the complete basis set CCSD(T) global minimum, respectively. These isomers were categorized into 15 different families based on their oxygen framework and hydrogen bonding topology. Determination of the global minimum proved challenging because of the presence of many nearly isoenergetic isomers. The predicted global minimum varied among ab initio methods, density functionals, and model potentials, and it was sensitive to the choice of energy extrapolation schemes, higher-order CCSD(T) corrections, and inclusion of zero-point vibrational energy. In conclusion, the presence of a large number of nearly degenerate structures and the isomerization between them has manifested itself in the anomalous broadening of the heat capacity curve of the undecamer in simulations around the melting region.},
doi = {10.1021/acs.jctc.7b00938},
journal = {Journal of Chemical Theory and Computation},
number = 2,
volume = 14,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 5 works
Citation information provided by
Web of Science

Save / Share:

Works referencing / citing this record:

Isomerism of the Aniline Trimer
journal, October 2018

  • Pérez, Cristóbal; León, Iker; Lesarri, Alberto
  • Angewandte Chemie International Edition, Vol. 57, Issue 46
  • DOI: 10.1002/anie.201808602