Why Is MP2-Water "Cooler" and "Denser" than DFT-Water?

The Journal of Physical Chemistry Letters
Soohaeng Yoo WillowSo Hirata

Abstract

Density functional theory (DFT) with a dispersionless generalized gradient approximation (GGA) needs much higher temperature and pressure than the ambient conditions to maintain water in the liquid phase at the correct (1 g/cm(3)) density during first-principles simulations. Conversely, ab initio second-order many-body perturbation (MP2) calculations of liquid water require lower temperature and pressure than DFT/GGA to keep water liquid. Here we present a unifying explanation of these trends derived from classical water simulations using a polarizable force field with different sets of parameters. We show that the different temperatures and pressures between DFT/GGA and MP2 at which the simulated water displays the experimentally observed liquid structure under the ambient conditions can be largely explained by their differences in polarizability and dispersion interaction, respectively. In DFT/GGA, the polarizability and thus the induced dipole moments and the hydrogen-bond strength are all overestimated. This hinders the rotational motion of molecules and requires a higher temperature for DFT-water to be liquid. MP2 gives a stronger dispersion interaction and thus shorter intermolecular distances than dispersionless DFT/GGA,...Continue Reading

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Citations

Mar 25, 2016·The Journal of Physical Chemistry. B·Yuki NagataMischa Bonn
May 18, 2016·Chemical Reviews·Gerardo Andrés CisnerosFrancesco Paesani
Jun 15, 2016·The Journal of Physical Chemistry. a·Maxim Tafipolsky
Mar 23, 2017·The Journal of Physical Chemistry Letters·Soohaeng Yoo Willow, Sotiris S Xantheas
May 23, 2017·Journal of Chemical Theory and Computation·Debashree MannaJan M L Martin
Aug 7, 2018·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Jian Liu, Sokrates T Pantelides
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May 19, 2020·Physical Chemistry Chemical Physics : PCCP·Soohaeng Yoo WillowDavid D L Minh
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Nov 11, 2019·The Journal of Chemical Physics·John M Herbert
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Apr 7, 2017·The Journal of Physical Chemistry. B·Chen Bai, Judith Herzfeld
Nov 22, 2018·Journal of Chemical Theory and Computation·Adam PhilipsJochen Autschbach

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