Error estimates for solid-state density-functional theory predictions: an overview by means of the ground-state elemental crystals

TL;DR

This paper reviews and quantifies the errors in density-functional theory predictions for elemental crystals, providing a practical protocol for estimating uncertainties in various material properties without additional calculations.

Contribution

It offers a comprehensive error analysis framework for DFT predictions based on a large test set, including reproducibility assessments across different computational methods.

Findings

Reproducibility of DFT predictions across methods is high, with a Delta factor of around 2-3 meV/atom.

Differences between PAW and APW+lo methods are negligible compared to experimental deviations.

The proposed protocol enables reliable error estimation for DFT predictions in materials research.

Abstract

Predictions of observable properties by density-functional theory calculations (DFT) are used increasingly often in experimental condensed-matter physics and materials engineering as data. These predictions are used to analyze recent measurements, or to plan future experiments. Increasingly more experimental scientists in these fields therefore face the natural question: what is the expected error for such an ab initio prediction? Information and experience about this question is scattered over two decades of literature. The present review aims to summarize and quantify this implicit knowledge. This leads to a practical protocol that allows any scientist - experimental or theoretical - to determine justifiable error estimates for many basic property predictions, without having to perform additional DFT calculations. A central role is played by a large and diverse test set of crystalline solids, containing all ground-state elemental crystals (except most lanthanides). For several properties of each crystal, the difference between DFT results and experimental values is assessed. We discuss trends in these deviations and review explanations suggested in the literature. A prerequisite for such an error analysis is that different implementations of the same first-principles formalism provide the same predictions. Therefore, the reproducibility of predictions across several mainstream methods and codes is discussed too. A quality factor Delta expresses the spread in predictions from two distinct DFT implementations by a single number. To compare the PAW method to the highly accurate APW+lo approach, a code assessment of VASP and GPAW with respect to WIEN2k yields Delta values of 1.9 and 3.3 meV/atom, respectively. These differences are an order of magnitude smaller than the typical difference with experiment, and therefore predictions by APW+lo and PAW are for practical purposes identical.