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Title: Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges

Nuclear quantum effects influence the structure and dynamics of hydrogen bonded systems, such as water, which impacts their observed properties with widely varying magnitudes. This review highlights the recent significant developments in the experiment, theory and simulation of nuclear quantum effects in water. Novel experimental techniques, such as deep inelastic neutron scattering, now provide a detailed view of the role of nuclear quantum effects in water’s properties. These have been combined with theoretical developments such as the introduction of the competing quantum effects principle that allows the subtle interplay of water’s quantum effects and their manifestation in experimental observables to be explained. We discuss how this principle has recently been used to explain the apparent dichotomy in water’s isotope effects, which can range from very large to almost nonexistent depending on the property and conditions. We then review the latest major developments in simulation algorithms and theory that have enabled the efficient inclusion of nuclear quantum effects in molecular simulations, permitting their combination with on-the-fly evaluation of the potential energy surface using electronic structure theory. Finally, we identify current challenges and future opportunities in the area.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [2] ;  [5] ;  [6]
  1. Ecole Polytechnique Federale Lausanne (Switzlerland)
  2. Univ. College London, Bloomsbury (United Kingdom)
  3. Univ. of Calgary, AB (Canada)
  4. Univ. of Queensland, Brisbane (Australia)
  5. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  6. Stanford Univ., Stanford, CA (United States)
Publication Date:
Report Number(s):
LLNL-JRNL-677797
Journal ID: ISSN 0009-2665
Grant/Contract Number:
AC05-00OR22725; AC52-07NA27344
Type:
Accepted Manuscript
Journal Name:
Chemical Reviews
Additional Journal Information:
Journal Volume: 116; Journal Issue: 13; Journal ID: ISSN 0009-2665
Publisher:
American Chemical Society
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1329776
Alternate Identifier(s):
OSTI ID: 1367996

Ceriotti, Michele, Fang, Wei, Kusalik, Peter G., Mckenzie, Ross H., Michaelides, Angelos, Morales, Miguel A., and Markland, Thomas E.. Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges. United States: N. p., Web. doi:10.1021/acs.chemrev.5b00674.
Ceriotti, Michele, Fang, Wei, Kusalik, Peter G., Mckenzie, Ross H., Michaelides, Angelos, Morales, Miguel A., & Markland, Thomas E.. Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges. United States. doi:10.1021/acs.chemrev.5b00674.
Ceriotti, Michele, Fang, Wei, Kusalik, Peter G., Mckenzie, Ross H., Michaelides, Angelos, Morales, Miguel A., and Markland, Thomas E.. 2016. "Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges". United States. doi:10.1021/acs.chemrev.5b00674. https://www.osti.gov/servlets/purl/1329776.
@article{osti_1329776,
title = {Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges},
author = {Ceriotti, Michele and Fang, Wei and Kusalik, Peter G. and Mckenzie, Ross H. and Michaelides, Angelos and Morales, Miguel A. and Markland, Thomas E.},
abstractNote = {Nuclear quantum effects influence the structure and dynamics of hydrogen bonded systems, such as water, which impacts their observed properties with widely varying magnitudes. This review highlights the recent significant developments in the experiment, theory and simulation of nuclear quantum effects in water. Novel experimental techniques, such as deep inelastic neutron scattering, now provide a detailed view of the role of nuclear quantum effects in water’s properties. These have been combined with theoretical developments such as the introduction of the competing quantum effects principle that allows the subtle interplay of water’s quantum effects and their manifestation in experimental observables to be explained. We discuss how this principle has recently been used to explain the apparent dichotomy in water’s isotope effects, which can range from very large to almost nonexistent depending on the property and conditions. We then review the latest major developments in simulation algorithms and theory that have enabled the efficient inclusion of nuclear quantum effects in molecular simulations, permitting their combination with on-the-fly evaluation of the potential energy surface using electronic structure theory. Finally, we identify current challenges and future opportunities in the area.},
doi = {10.1021/acs.chemrev.5b00674},
journal = {Chemical Reviews},
number = 13,
volume = 116,
place = {United States},
year = {2016},
month = {4}
}