Hubbard corrections from first-principles made easy via automated and reproducible workflows

Hubbard-corrected density-functional theory in its extended formulation (DFT+U+V) has proven to accurately capture the electronic structure and physical properties of compounds containing localized d and f electrons [1], greatly reducing self-interaction errors. While the onsite (U) and intersite (V) Hubbard parameters can be computed self-consistently from first-principles, their large-scale determination necessitates a robust and scalable approach. Here, we present an automated, flexible framework based on the AiiDA infrastructure to self-consistently calculate these parameters using density-functional perturbation theory [2]. We demonstrate the scalability and reliability of the framework by computing in a high-throughput fashion the self-consistent onsite U and intersite V parameters for 115 Li-containing bulk solids with up to 32 atoms. Our analysis of the computed Hubbard parameters reveals a significant correlation of the onsite U values on the oxidation state and coordination environment of the central atom, while intersite V values exhibit a general decay with increasing interatomic distance. This framework paves the way for high-throughput screening across diverse research areas, including the discovery of novel cathode materials for Li-ion batteries, as well as other technologically-relevant applications.



[1] I. Timrov et al., PRX Energy 1, 033003 (2022)

[2] I. Timrov et al., PRB 98, 085127 (2018)