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

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

Abstract

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:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Stanford Univ., CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1329776
Alternate Identifier(s):
OSTI ID: 1367996; OSTI ID: 1526758
Report Number(s):
LLNL-JRNL-677797
Journal ID: ISSN 0009-2665
Grant/Contract Number:  
AC05-00OR22725; AC52-07NA27344; SC0014437
Resource 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
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; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Quantum mechanics, aqueous systems, water

Citation Formats

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., 2016. 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. Wed . "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}
}

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

Citation Metrics:
Cited by: 58 works
Citation information provided by
Web of Science

Save / Share:

Works referencing / citing this record:

Unraveling the structural and chemical features of biological short hydrogen bonds
journal, January 2019


Self-diffusion coefficient of bulk and confined water: a critical review of classical molecular simulation studies
journal, August 2018

  • Tsimpanogiannis, Ioannis N.; Moultos, Othonas A.; Franco, Luís F. M.
  • Molecular Simulation, Vol. 45, Issue 4-5
  • DOI: 10.1080/08927022.2018.1511903

Emerging hydrovoltaic technology
journal, December 2018


Streams, cascades, and pools: various water cluster motifs in structurally similar Ni( ii ) complexes
journal, January 2018

  • Saraei, Nina; Hietsoi, Oleksandr; Mullins, Christopher S.
  • CrystEngComm, Vol. 20, Issue 44
  • DOI: 10.1039/c8ce01153b

Emerging hydrovoltaic technology
journal, December 2018


Streams, cascades, and pools: various water cluster motifs in structurally similar Ni( ii ) complexes
journal, January 2018

  • Saraei, Nina; Hietsoi, Oleksandr; Mullins, Christopher S.
  • CrystEngComm, Vol. 20, Issue 44
  • DOI: 10.1039/c8ce01153b

Quantum tunnelling pathways of the water pentamer
journal, January 2020

  • Cvitaš, Marko T.; Richardson, Jeremy O.
  • Physical Chemistry Chemical Physics, Vol. 22, Issue 3
  • DOI: 10.1039/c9cp05561d

Unraveling the structural and chemical features of biological short hydrogen bonds
journal, January 2019


Nuclear quantum effects on the vibrational dynamics of liquid water
journal, March 2018

  • Ojha, Deepak; Henao, Andrés; Kühne, Thomas D.
  • The Journal of Chemical Physics, Vol. 148, Issue 10
  • DOI: 10.1063/1.5005500

Stabilization of ammonia-rich hydrate inside icy planets
journal, August 2017

  • Naden Robinson, Victor; Wang, Yanchao; Ma, Yanming
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 34
  • DOI: 10.1073/pnas.1706244114

Self-diffusion coefficient of bulk and confined water: a critical review of classical molecular simulation studies
journal, August 2018

  • Tsimpanogiannis, Ioannis N.; Moultos, Othonas A.; Franco, Luís F. M.
  • Molecular Simulation, Vol. 45, Issue 4-5
  • DOI: 10.1080/08927022.2018.1511903