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Reproducibility of density functional approximations: How new functionals should be reported
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DOI：10.1063/5.0167763.png)
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Abstract
En 中文
Density functional theory is the workhorse of chemistry and materials science, and novel density functional approximations are published every year. To become available in program packages, the novel density functional approximations (DFAs) need to be (re)implemented.However, according to our experience as developers of Libxc [Lehtolaet al., SoftwareX7, 1 (2018)], a constant problem in this task is verification due to the lack of reliable reference data. As we discuss in this work, this lack has led to several non-equivalent implementationsof functionals such as Becke-Perdew 1986, Perdew-Wang 1991, Perdew-Burke-Ernzerhof, and Becke's three-parameter hybrid functionalwith Lee-Yang-Parr correlation across various program packages, yielding different total energies. Through careful verification, we have alsofound many issues with incorrect functional forms in recent DFAs. The goal of this work is to ensure the reproducibility of DFAs. DFAsmust be verifiable in order to prevent the reappearance of the above-mentioned errors and incompatibilities. A common framework for ver-ification and testing is, therefore, needed. We suggest several ways in which reference energies can be produced with free and open sourcesoftware, either with non-self-consistent calculations with tabulated atomic densities or via self-consistent calculations with various programpackages. The employed numerical parameters-especially the quadrature grid-need to be converged to guarantee a less than or similar to 0.1 mu E(h)precision inthe total energy, which is nowadays routinely achievable in fully numerical calculations. Moreover, as such sub-mu E(h)level agreement can onlybe achieved when fully equivalent implementations of the DFA are used, the source code of the reference implementation should also be madeavailable in any publication describing a new DFA
Keywords:
GENERALIZED GRADIENT APPROXIMATION
GAUSSIAN-BASIS SETS
FOCK WAVE-FUNCTIONS
CORRELATION-ENERGY
BROAD ACCURACY
ELECTRONIC-STRUCTURE
EXCHANGE
HYBRID
ATOMS
THERMOCHEMISTRY
Journal
IF:
3.1
Papers:
7.2W
Citations:
23.2W