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

• Published in: arXiv.org 2023-05
• Main Authors: Bosoni, Emanuele, Beal, Louis, Bercx, Marnik, Blaha, Peter, Blügel, Stefan, Bröder, Jens, Callsen, Martin, Cottenier, Stefaan, Degomme, Augustin, Dikan, Vladimir, Eimre, Kristjan, Flage-Larsen, Espen, nari, Marco, Garcia, Alberto, Genovese, Luigi, Giantomassi, Matteo, Huber, Sebastiaan P, Janssen, Henning, Kastlunger, Georg, Krack, Matthias, Kresse, Georg, Kühne, Thomas D, Lejaeghere, Kurt, Madsen, Georg K H, Marsman, Martijn, Marzari, Nicola, Michalicek, Gregor, Mirhosseini, Hossein, Müller, Tiziano M A, Petretto, Guido, Pickard, Chris J, Poncé, Samuel, Gian-Marco Rignanese, Rubel, Oleg, Ruh, Thomas, Sluydts, Michael, Vanpoucke, Danny E P, Sudarshan Vijay, Wolloch, Michael, Wortmann, Daniel, Yakutovich, Aliaksandr V, Yu, Jusong, Austin Zadoks, Zhu, Bonan, Pizzi, Giovanni
• Format: Article
• Language: English
• Subjects: Boundary conditions; Condensed matter physics; Coordination numbers; Density functional theory; Equations of state; Free energy; Heat of formation; Materials science; Oxidation; Periodic table; Reliability analysis; Reproducibility
• ISSN: 2331-8422
• DOI: 10.48550/arxiv.2305.17274

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).