MN15-L: A New Local Exchange-Correlation Functional for Kohn-Sham Density Functional Theory with Broad Accuracy for Atoms, Molecules, and Solids

Haoyu S. Yu, Xiao He, Donald G Truhlar

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161 Scopus citations

Abstract

Kohn-Sham density functional theory is widely used for applications of electronic structure theory in chemistry, materials science, and condensed-matter physics, but the accuracy depends on the quality of the exchange-correlation functional. Here, we present a new local exchange-correlation functional called MN15-L that predicts accurate results for a broad range of molecular and solid-state properties including main-group bond energies, transition metal bond energies, reaction barrier heights, noncovalent interactions, atomic excitation energies, ionization potentials, electron affinities, total atomic energies, hydrocarbon thermochemistry, and lattice constants of solids. The MN15-L functional has the same mathematical form as a previous meta-nonseparable gradient approximation exchange-correlation functional, MN12-L, but it is improved because we optimized it against a larger database, designated 2015A, and included smoothness restraints; the optimization has a much better representation of transition metals. The mean unsigned error on 422 chemical energies is 2.32 kcal/mol, which is the best among all tested functionals, with or without nonlocal exchange. The MN15-L functional also provides good results for test sets that are outside the training set. A key issue is that the functional is local (no nonlocal exchange or nonlocal correlation), which makes it relatively economical for treating large and complex systems and solids. Another key advantage is that medium-range correlation energy is built in so that one does not need to add damped dispersion by molecular mechanics in order to predict accurate noncovalent binding energies. We believe that the MN15-L functional should be useful for a wide variety of applications in chemistry, physics, materials science, and molecular biology.

Original languageEnglish (US)
Pages (from-to)1280-1293
Number of pages14
JournalJournal of Chemical Theory and Computation
Volume12
Issue number3
DOIs
StatePublished - Mar 8 2016

Bibliographical note

Funding Information:
The authors are grateful to Wei-Guang Liu, Pragya Verma, Jingjing Zheng, and Kaining Duanmu for very helpful assistance. H.Y. acknowledges support by a Doctoral Dissertation Fellowship. This work was also supported in part by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences under Award DESC0012702 to the Inorganometallic Catalyst Design Center and by using Molecular Science Computing Facility in William R. Wiley Environmental Molecular Sciences Laboratory of Pacific Northwest National Laboratory sponsored by the U. S. Department of Energy.

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