The quest for a universal density functional: The accuracy of density\n functionals across a broad spectrum of databases in chemistry and physics

2012/12/05 by Roberto Peverati, Donald G. Truhlar, Peverati, Roberto +1
Chemical Engineering · Materials Science · Physics and Astronomy · #Advanced Chemical Physics Studies #Catalysis and Oxidation Reactions #Chemical Physics (physics.chem-ph) #Computational Physics (physics.comp-ph) #FOS: Physical sciences #Machine Learning in Materials Science #Materials Science (cond-mat.mtrl-sci) #Quantum Physics (quant-ph)

paper · pdf · doi:10.48550/arxiv.1212.0944

openalex publication_date 2012/12/05 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28

Abstract

Kohn-Sham density functional theory is in principle an exact formulation of\nquantum mechanical electronic structure theory, but in practice we have to rely\non approximate exchange-correlation (xc) functionals. The objective of our work\nhas been to design an xc functional with broad accuracy across as wide an\nexpanse of chemistry and physics as possible, leading-as a long-range goal-to a\nfunctional with good accuracy for all problems, i.e., a universal functional.\nTo guide our path toward that goal and to measure our progress, we have\ndeveloped-building on earlier work in our group-a set of databases of reference\ndata for a variety of energetic and structural properties in chemistry and\nphysics. These databases include energies of molecular processes such as\natomization, complexation, proton addition, and ionization; they also include\nmolecular geometries and solid-state lattice constants, chemical reaction\nbarrier heights, and cohesive energies and band gaps of solids. For the present\npaper we gather many of these databases into four comprehensive databases, two\nwith 384 energetic data for chemistry and solid-state physics and another two\nwith 68 structural data for chemistry and solid-state physics, and we test 2\nwave function methods and 77 density functionals (12 Minnesota meta functionals\nand 65 others) in a consistent way across this same broad set of data. We\nespecially highlight the Minnesota density functionals, but the results have\nbroader implications in that one may see the successes and failures of many\nkinds of density functionals when they are all applied to the same data.\nTherefore the results provide a status report on the quest for a universal\nfunctional.\n

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