Abstract
Understanding the applicability and limitations of electronic-structure methods needs careful and efficient comparison with accurate reference data. Knowledge of the quality and errors of electronic-structure calculations is crucial to advanced method development, high-throughput computations and data analyses. In this paper, we present a main-group test set for computational materials science and engineering (MSE), that provides accurate and easily accessible crystal properties for a hierarchy of exchange-correlation approximations, ranging from the well-established mean-field approximations to the state-of-the-art methods of many-body perturbation theory. We consider cohesive energy, lattice constant and bulk modulus of a set of materials that representatives for the first- and second-row elements and their binaries with cubic crystal structures and various bonding characters. A strong effort is made to achieve high numerical accuracy for cohesive properties as calculated using the local-density approximation (LDA), several generalized gradient approximations (GGAs), meta-GGAs and hybrids in all-electron resolution, and the second-order Møller–Plesset perturbation theory (MP2) and the random-phase approximation (RPA) both with frozen-core approximation based on all-electron Hartree–Fock, PBE and/or PBE0 references. This results in over 10 000 calculations, which record a comprehensive convergence test with respect to numerical parameters for a wide range of electronic-structure methods within the numerical atom-centered orbital framework. As an indispensable part of the MSE test set, a web site is established http://mse.fhi-berlin.mpg.de. This not only allows for easy access to all reference data but also provides user-friendly graphical tools for post-processing error analysis.
Highlights
First-principles electronic-structure calculations have become an indispensable complement to experiments in physics, chemistry, and materials science, etc
A strong effort is made to push the borders of numerical accuracy for cohesive properties as calculated using the local-density approximation (LDA), several generalized gradient approximations (GGAs), meta-GGAs and hybrids in all-electron resolution, and the second-order Møller-Plesset perturbation theory (MP2) and the random-phase approximation (RPA) with frozen-core approximation based on all-electron Hartree-Fock, PBE and/or PBE0 references
We argue that the performance of the complete basis set (CBS)(3,4) strategy in molecules is transferable to solids, which can be used to converge the RPA and MP2 total energies per atom in the materials science and engineering (MSE) test set with a similar numerical uncertainty on average
Summary
First-principles electronic-structure calculations have become an indispensable complement to experiments in physics, chemistry, and materials science, etc. In quantum chemistry for atoms and molecules, test sets with accurate reference values for various relevant chemical and physical properties have been since long established [1,2,3,4,5,6,7,8,9,10,11,12,13,14,15] These test sets play an instrumental role in the development of hierarchical electronicstructure approximations for both wave-function theory (WFT) and density-functional theory (DFT). The paper is structured as follows: After a detailed survey of the test sets that are widely used in quantum chemistry, as well as in materials science, we discuss the underlying challenges to obtain numerically accurate reference data in the latter.
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