Pair your accounts.

Export articles to Mendeley

Get article recommendations from ACS based on references in your Mendeley library.

Pair your accounts.

Export articles to Mendeley

Get article recommendations from ACS based on references in your Mendeley library.

You’ve supercharged your research process with ACS and Mendeley!

STEP 1:
Click to create an ACS ID

Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

MENDELEY PAIRING EXPIRED
Your Mendeley pairing has expired. Please reconnect
ACS Publications. Most Trusted. Most Cited. Most Read
Determining Partial Atomic Charges for Liquid Water: Assessing Electronic Structure and Charge Models

OR SEARCH CITATIONS

My Activity
Publications
CONTENT TYPES

Figure 1Loading Img
Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Chem. Theory Comput. 2021, 17, 2, 889-901
    Quantum Electronic Structure

    Determining Partial Atomic Charges for Liquid Water: Assessing Electronic Structure and Charge Models
    Click to copy article linkArticle link copied!

    Other Access OptionsSupporting Information (1)

    Journal of Chemical Theory and Computation

    Cite this: J. Chem. Theory Comput. 2021, 17, 2, 889–901
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jctc.0c01102
    Published January 6, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

    Abstract

    Click to copy section linkSection link copied!
    Abstract Image

    Partial atomic charges provide an intuitive and efficient way to describe the charge distribution and the resulting intermolecular electrostatic interactions in liquid water. Many charge models exist and it is unclear which model provides the best assignment of partial atomic charges in response to the local molecular environment. In this work, we systematically scrutinize various electronic structure methods and charge models (Mulliken, natural population analysis, CHelpG, RESP, Hirshfeld, Iterative Hirshfeld, and Bader) by evaluating their performance in predicting the dipole moments of isolated water, water clusters, and liquid water as well as charge transfer in the water dimer and liquid water. Although none of the seven charge models is capable of fully capturing the dipole moment increase from isolated water (1.85 D) to liquid water (about 2.9 D), the Iterative Hirshfeld method performs best for liquid water, reproducing its experimental average molecular dipole moment, yielding a reasonable amount of intermolecular charge transfer, and showing modest sensitivity to the local water environment. The performance of the charge model is dependent on the choice of the density functional and the quantum treatment of the environment. The computed molecular dipole moment of water generally increases with the percentage of the exact Hartree–Fock exchange in the functional, whereas the amount of charge transfer between molecules decreases. For liquid water, including two full solvation shells of surrounding water molecules (within about 5.5 Å of the central water) in the quantum chemical calculation converges the charges of the central water molecule. Our final pragmatic quantum chemical charge-assigning protocol for liquid water is the Iterative Hirshfeld method with M06-HF/aug-cc-pVDZ and a quantum region cutoff radius of 5.5 Å.

    Copyright © 2021 American Chemical Society

    Subjects

    what are subjects

    Read this article

    To access this article, please review the available access options below.

    Get instant access

    Purchase Access

    Read this article for 48 hours. Check out below using your ACS ID or as a guest.

    Recommended

    Access through Your Institution

    You may have access to this article through your institution.

    Your institution does not have access to this content. Add or change your institution or let them know you’d like them to include access.

    Supporting Information

    Click to copy section linkSection link copied!

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jctc.0c01102.

    • Structures of water clusters; calculated partial atomic charges, molecular dipoles, and net charges if there is charge transfer, for isolated water, water clusters, and liquid water using various quantum chemical methods and charge models; and comparison of these results (PDF)

    Terms & Conditions

    Electronic Supporting Information files are available without a subscription to ACS Web Editions. The American Chemical Society holds a copyright ownership interest in any copyrightable Supporting Information. Files available from the ACS website may be downloaded for personal use only. Users are not otherwise permitted to reproduce, republish, redistribute, or sell any Supporting Information from the ACS website, either in whole or in part, in either machine-readable form or any other form without permission from the American Chemical Society. For permission to reproduce, republish and redistribute this material, requesters must process their own requests via the RightsLink permission system. Information about how to use the RightsLink permission system can be found at http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    Click to copy section linkSection link copied!

    This article is cited by 18 publications.

    1. Fabio Biffoli, Davide Vanossi, Elisabetta Venuti, Tommaso Salzillo, Marco Bonechi, Massimo Innocenti, Marco Pagliai, Claudio Fontanesi. Charge Transfer in Molecular Cocrystals: A Plane Wave vs Localized-Orbital View─Structural Information Obtained from Calculated Raman and IR Phonons. The Journal of Physical Chemistry C 2024, 128 (33) , 14046-14055. https://doi.org/10.1021/acs.jpcc.4c03470
    2. Andrey V. Solov’yov, Alexey V. Verkhovtsev, Nigel J. Mason, Richard A. Amos, Ilko Bald, Gérard Baldacchino, Brendan Dromey, Martin Falk, Juraj Fedor, Luca Gerhards, Michael Hausmann, Georg Hildenbrand, Miloš Hrabovský, Stanislav Kadlec, Jaroslav Kočišek, Franck Lépine, Siyi Ming, Andrew Nisbet, Kate Ricketts, Leo Sala, Thomas Schlathölter, Andrew E. H. Wheatley, Ilia A. Solov’yov. Condensed Matter Systems Exposed to Radiation: Multiscale Theory, Simulations, and Experiment. Chemical Reviews 2024, 124 (13) , 8014-8129. https://doi.org/10.1021/acs.chemrev.3c00902
    3. Kyana M. Sanders, Jonathan S. Van Buskirk, Katerina P. Hilleke, Daniel C. Fredrickson. Self-Consistent Chemical Pressure Analysis: Resolving Atomic Packing Effects through the Iterative Partitioning of Space and Energy. Journal of Chemical Theory and Computation 2023, 19 (13) , 4273-4285. https://doi.org/10.1021/acs.jctc.3c00368
    4. Bowen Han, Christine M. Isborn, Liang Shi. Incorporating Polarization and Charge Transfer into a Point-Charge Model for Water Using Machine Learning. The Journal of Physical Chemistry Letters 2023, 14 (16) , 3869-3877. https://doi.org/10.1021/acs.jpclett.3c00036
    5. Philipp Schienbein. Spectroscopy from Machine Learning by Accurately Representing the Atomic Polar Tensor. Journal of Chemical Theory and Computation 2023, 19 (3) , 705-712. https://doi.org/10.1021/acs.jctc.2c00788
    6. Christina Ertural, Ralf P. Stoffel, Peter C. Müller, C. Alexander Vogt, Richard Dronskowski. First-Principles Plane-Wave-Based Exploration of Cathode and Anode Materials for Li- and Na-Ion Batteries Involving Complex Nitrogen-Based Anions. Chemistry of Materials 2022, 34 (2) , 652-668. https://doi.org/10.1021/acs.chemmater.1c03349
    7. Francisco Ballesteros, Ka Un Lao. Accelerating the Convergence of Self-Consistent Field Calculations Using the Many-Body Expansion. Journal of Chemical Theory and Computation 2022, 18 (1) , 179-191. https://doi.org/10.1021/acs.jctc.1c00765
    8. Kathryn Walden, Madison E. Martin, Lacey LaBee, Makenzie Provorse Long. Hydration and Charge-Transfer Effects of Alkaline Earth Metal Ions Binding to a Carboxylate Anion, Phosphate Anion, and Guanine Nucleobase. The Journal of Physical Chemistry B 2021, 125 (44) , 12135-12146. https://doi.org/10.1021/acs.jpcb.1c05757
    9. Janus J. Eriksen. Decomposed Mean-Field Simulations of Local Properties in Condensed Phases. The Journal of Physical Chemistry Letters 2021, 12 (26) , 6048-6055. https://doi.org/10.1021/acs.jpclett.1c01375
    10. Huanquan Cheng, Longgui Peng, Jia Liu, Cuiying Ma, Fangtao Hao, Bin Zheng, Jianye Yang. Adsorption Separation of Various Polar Dyes in Water by Oil Sludge-Based Porous Carbon. Applied Sciences 2024, 14 (16) , 7283. https://doi.org/10.3390/app14167283
    11. Hajime Torii. Roles of electrostatics and intermolecular electronic motions in the structural and spectroscopic features of hydrogen- and halogen-bonded systems. Pure and Applied Chemistry 2024, 96 (4) , 579-595. https://doi.org/10.1515/pac-2023-1202
    12. Olivier Bouty. Reaction mechanisms in hydrated magnesium silicate glass investigated by Ab-Initio methods and Metadynamics. Computational Materials Science 2024, 232 , 112632. https://doi.org/10.1016/j.commatsci.2023.112632
    13. Mohsen Sotoudeh, Sebastian Baumgart, Manuel Dillenz, Johannes Döhn, Katrin Forster‐Tonigold, Katharina Helmbrecht, Daniel Stottmeister, Axel Groß. Ion Mobility in Crystalline Battery Materials. Advanced Energy Materials 2024, 14 (4) https://doi.org/10.1002/aenm.202302550
    14. M.B. Kiataki, M.T. do N. Varella, K. Coutinho. New approach to instantaneous polarizable electrostatic embedding of the solvent. Journal of Molecular Liquids 2023, 389 , 122861. https://doi.org/10.1016/j.molliq.2023.122861
    15. Asma Hassan, Muhammad Ismail, Ali H. Reshak, Zeshan Zada, Abdul Ahad Khan, Fazal Ur Rehman M, Muhammad Arif, Khadija Siraj, Shafqat Zada, G. Murtaza, Muhammad M. Ramli. Effect of heteroatoms on structural, electronic and spectroscopic properties of polyfuran, polythiophene and polypyrrole: A hybrid DFT approach. Journal of Molecular Structure 2023, 1274 , 134484. https://doi.org/10.1016/j.molstruc.2022.134484
    16. B.B. Xiao, Z. Zhang, L.B. Yu, Q.Y. Huang, J. Wu, E.H. Song, L.L. Wang. Boosting oxygen reduction electrocatalysis of graphene-based bilayer heterojunction. Surfaces and Interfaces 2022, 33 , 102232. https://doi.org/10.1016/j.surfin.2022.102232
    17. Hasnia Abdeldjebar, Chafia Ait-Ramdane-Terbouche, Achour Terbouche, Houria Lakhdari. Exploring Schiff base ligand inhibitor for cancer and neurological cells, viruses and bacteria receptors by homology modeling and molecular docking. Computational Toxicology 2022, 23 , 100231. https://doi.org/10.1016/j.comtox.2022.100231
    18. Oliver R. Gittus, Fernando Bresme. Thermophysical properties of water using reactive force fields. The Journal of Chemical Physics 2021, 155 (11) https://doi.org/10.1063/5.0057868
    Download PDF
    Go to Journal of Chemical Theory and Computation
    Get e-Alerts
    Get e-Alerts

    Journal of Chemical Theory and Computation

    Cite this: J. Chem. Theory Comput. 2021, 17, 2, 889–901
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jctc.0c01102
    Published January 6, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

    Article Views

    1580

    Altmetric

    -

    Citations

    18
    Learn about these metrics

    Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.

    Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.

    The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.