How to verify the precision of density-functional-theory implementations via reproducible and universal workflows

Abstract

In the past decades many density-functional theory methods and codes adopting periodic boundary conditions have been developed and are now extensively used in condensed matter physics and materials science research. Only in 2016, however, their precision (i.e., to which extent properties computed with different codes agree among each other) was systematically assessed on elemental crystals: a first crucial step to evaluate the reliability of such computations. We discuss here general recommendations for verification studies aiming at further testing precision and transferability of density-functional-theory computational approaches and codes. We illustrate such recommendations using a greatly expanded protocol covering the whole periodic table from Z=1 to 96 and characterizing 10 prototypical cubic compounds for each element: 4 unaries and 6 oxides, spanning a wide range of coordination numbers and oxidation states. The primary outcome is a reference dataset of 960 equations of state cross-checked between two all-electron codes, then used to verify and improve nine pseudopotential-based approaches. Such effort is facilitated by deploying AiiDA common workflows that perform automatic input parameter selection, provide identical input/output interfaces across codes, and ensure full reproducibility. Finally, we discuss the extent to which the current results for total energies can be reused for different goals (e.g., obtaining formation energies).

Main text: 23 pages, 4 figures. Supplementary: 68 pages. Nature Review Physics 2023

References in corpus (3)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• SIESTA: recent developments and applications

Cited by in corpus (20)

• JARVIS-Leaderboard: A Large Scale Benchmark of Materials Design Methods
• Abinit 2025: New Capabilities for the Predictive Modeling of Solids and Nanomaterials
• The Wannier Function Software Ecosystem for Materials Simulations
• Quantum Simulations of Chemistry in First Quantization with any Basis Set
• Verification and Validation of zero-point electron-phonon renormalization of the bandgap, mass enhancement, and spectral functions
• Phonons from Density-Functional Perturbation Theory using the All-Electron Full-Potential Linearized Augmented Plane-Wave Method FLEUR
• First-principles Hubbard parameters with automated and reproducible workflows
• The impact of strain on the GeV-color center in diamond
• Reproducibility of fixed-node diffusion Monte Carlo across diverse community codes: The case of water-methane dimer
• Quantum Computation of Electronic Structure with Projector Augmented-Wave Method and Plane Wave Basis Set
• Automated computational workflows for muon spin spectroscopy
• MC3D: The Materials Cloud computational database of experimentally known stoichiometric inorganics
• Trimeron ordering, bandgap and polaron hopping in magnetite
• MADAS -- A Python framework for assessing similarity in materials-science data
• Teaching oxidation states to neural networks
• Algorithmic differentiation for plane-wave DFT: materials design, error control and learning model parameters
• Impact of Exchange-Correlation Functionals on Predictions of Phonon Hydrodynamics: A Study of Fluorides, Chlorides, and Hydrides
• Making atomistic materials calculations accessible with the AiiDAlab Quantum ESPRESSO app
• A Denser Hydrogen Inferred from First-Principles Simulations Challenges Jupiter's Interior Models
• Modeling the Zero-Phonon Line of Strained SnV Centers in Diamond; Including Reflections on Computational Cost and Accuracy