Accessing the accuracy of density functional theory through structure and dynamics of the water-air interface
Ohto T, Dodia M, Xu J, Imoto S, Tang F, Zysk F, Kühne TD, Shigeta Y, Bonn M, Wu X, Nagata Y (2019)
Publication Type: Journal article
Publication year: 2019
Journal
Book Volume: 10
Pages Range: 4914-4919
Journal Issue: 17
DOI: 10.1021/acs.jpclett.9b01983
Abstract
Density functional theory-based molecular dynamics simulations are increasingly being used for simulating aqueous interfaces. Nonetheless, the choice of the appropriate density functional, critically affecting the outcome of the simulation, has remained arbitrary. Here, we assess the performance of various exchange-correlation (XC) functionals, based on the metrics relevant to sum-frequency generation spectroscopy. The structure and dynamics of water at the water-air interface are governed by heterogeneous intermolecular interactions, thereby providing a critical benchmark for XC functionals. We find that the XC functionals constrained by exact functional conditions (revPBE and revPBE0) with the dispersion correction show excellent performance. The poor performance of the empirically optimized density functional (M06-L) indicates the importance of satisfying the exact functional condition. Understanding the performance of different XC functionals can aid in resolving the controversial interpretation of the interfacial water structure and direct the design of novel, improved XC functionals better suited to describing the heterogeneous interactions in condensed phases.
Involved external institutions
Osaka University
Japan (JP)
Temple University
United States (USA) (US)
Max-Planck-Institut für Polymerforschung (MPI-P) / Max Planck Institute for Polymer Research
Germany (DE)
Universität Paderborn
Germany (DE)
University of Tsukuba / 筑波大学
Japan (JP)
Japan (JP)
Temple University
United States (USA) (US)
Max-Planck-Institut für Polymerforschung (MPI-P) / Max Planck Institute for Polymer Research
Germany (DE)
Universität Paderborn
Germany (DE)
University of Tsukuba / 筑波大学
Japan (JP)
How to cite
APA:
Ohto, T., Dodia, M., Xu, J., Imoto, S., Tang, F., Zysk, F.,... Nagata, Y. (2019). Accessing the accuracy of density functional theory through structure and dynamics of the water-air interface. Journal of Physical Chemistry Letters, 10(17), 4914-4919. https://doi.org/10.1021/acs.jpclett.9b01983
MLA:
Ohto, Tatsuhiko, et al. "Accessing the accuracy of density functional theory through structure and dynamics of the water-air interface." Journal of Physical Chemistry Letters 10.17 (2019): 4914-4919.
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