Optimization of an exchange-correlation density functional for water

We describe a method, that we call data projection onto parameter space (DPPS), to optimize an energy functional of the electron density, so that it reproduces a dataset of experimental magnitudes. Our scheme, based on Bayes theorem, constrains the optimized functional not to depart unphysically fro...

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Veröffentlicht in:arXiv.org 2016-03
Hauptverfasser: Fritz, Michelle, Fernandez-Serra, Marivi, Soler, Jose M
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description We describe a method, that we call data projection onto parameter space (DPPS), to optimize an energy functional of the electron density, so that it reproduces a dataset of experimental magnitudes. Our scheme, based on Bayes theorem, constrains the optimized functional not to depart unphysically from existing ab initio functionals. The resulting functional maximizes the probability of being the \correct" parametrization of a given functional form, in the sense of Bayes theory. The application of DPPS to water sheds new light on why density functional theory has performed rather poorly for liquid water, on what improvements are needed, and on the intrinsic limitations of the generalized gradient approximation to electron exchange and correlation. Finally, we present tests of our water-optimized functional, that we call vdW-DF-w, showing that it performs very well for a variety of condensed water systems.
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subjects Bayes Theorem
Bayesian analysis
Density functional theory
Electron density
Exchanging
Optimization
Parameterization
Physics - Chemical Physics
Physics - Computational Physics
Physics - Other Condensed Matter
Water
title Optimization of an exchange-correlation density functional for water
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