Accessing the Accuracy of Density Functional Theory through Structure and Dynamics of the Water-Air Interface

The Journal of Physical Chemistry Letters
Tatsuhiko OhtoYuki Nagata

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.

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Citations

Apr 10, 2020·The Journal of Chemical Physics·Tatsuya Ishiyama
May 13, 2020·Proceedings of the National Academy of Sciences of the United States of America·Kamal SharkasJuan E Peralta
Sep 3, 2020·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Deepak Ojha, Thomas D Kühne
Jul 7, 2021·Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology·Ferdinand L KissStefano Crespi
Dec 14, 2019·The Journal of Physical Chemistry Letters·Ruiyu WangEric Borguet
Dec 24, 2019·Journal of the American Chemical Society·Sudipta DasMischa Bonn
Sep 16, 2021·The Journal of Physical Chemistry Letters·Sam ShepherdVenkat Kapil
Oct 14, 2021·Physical Chemistry Chemical Physics : PCCP·Takaya OgawaTakeo Yamaguchi

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