Quest for a universal density functional: the accuracy of density functionals across a broad spectrum of databases in chemistry and physics

By Roberto Peverati, Donald G. Truhlar. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, 2012

662 citations recorded by the source corpus.

Kohn–Sham density functional theory is in principle an exact formulation of quantum mechanical electronic structure theory, but in practice we have to rely on approximate exchange–correlation (xc) functionals. The objective of our work has been to design an xc functional with broad accuracy across as wide an expanse of chemistry and physics as possible, leading—as a long-range goal—to a functional with good accuracy for all problems, i.e. a universal functional. To guide our path towards that goal and to measure our progress, we have developed—building on earlier work of our group—a set of databases of reference data for a variety of energetic and structural properties in chemistry and physics. These databases include energies of molecular processes, such as atomization, complexation, proton addition and ionization; they also include molecular geometries and solid-state lattice constants, chemical reaction barrier heights, and cohesive energies and band gaps of solids. For this paper, we gather many of these databases into four comprehensive databases, two with 384 energetic data for chemistry and solid-state physics and another two with 68 structural data for chemistry and solid-state physics, and we test two wave function methods and 77 density functionals (12 Minnesota meta functionals and 65 others) in a consistent way across this same broad set of data. We especially highlight the Minnesota density functionals, but the results have broader implications in that one may see the successes and failures of many kinds of density functionals when they are all applied to the same data. Therefore, the results provide a status report on the quest for a universal functional.

Subfields: Atomic and Molecular Physics, and Optics, Catalysis, Materials Chemistry

View Paper: https://www.semanticscholar.org/paper/835fe7982211bad06a03b29d1447cd6228a4c9da

How researchers see this paper

The researchers whose trusted networks rank it highest, strongest advocate first. Every researcher gets a different order.

In Atomic and Molecular Physics, and Optics

1. Lars Goerigk
2. Stefan Grimme
3. Tanmoy Das
4. Hsin Lin
5. Arun Bansil
6. Donald G. Truhlar
7. Roberto Peverati
8. Tian Lu

In Catalysis

1. Stefan Grimme
2. Lars Goerigk

In Materials Chemistry

1. Tanmoy Das
2. Stefan Grimme
3. Lars Goerigk
4. Hsin Lin
5. Arun Bansil
6. Simon Axelrod
7. Rafael Gómez‐Bombarelli

Citations in the corpus

• Colloquium : Topological band theory (2016, background): “(Peverati and Truhlar 2014; Capelle and Campo Jr. 2013; Held et al. 2006; Maier et al. 2005; Kotliar et al. 2006; Das, Markiewicz, and Bansil 2014) It is natural to expect that the combined effects of strong correlations and SOC would give rise to entirely new classes of TIs.”
• Status and Challenges of Density Functional Theory (2020, neutral): “Next we discuss the performance of the following density functionals on the NCCE30/18 [35–42], MR-TMD-BE3 [38,43], DGL6 [35,38], TMDBL10 [44], and TSG48 [45] databases, which are part of Minnesota Database 2019: • GAs: PBE [30], GAM [38] • meta approximations: M06-L [32], revM06-L [46], MN15-L [47] ”
• Double‐hybrid density functionals (2014, background): “If this ansatz is expanded in the usual way, the following first two energy terms of the series are obtained from the KS reference determinant Φs as E0 + E1 = Ts + Eext + J + Ex, (2)”