Lorenzo Bastonero^1*, Cristiano Malica¹, Eric Macke¹, Marnik Bercx², Sebastian P. Huber³, Iurii Timrov², Nicola Marzari^1,2,3

1 U Bremen Excellence Chair, Bremen Center for Computational Materials Science, and MAPEX Center for Materials and Processes, University of Bremen, D-28359 Bremen, Germany

2 PSI Center for Scientific Computing, Theory, and Data, and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), 5232 Villigen PSI, Switzerland

3 Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

* Corresponding authors emails: lbastone@uni-bremen.de

DOI10.24435/materialscloud:v2-60 [version v1]

Publication date: Feb 27, 2025

How to cite this record

Lorenzo Bastonero, Cristiano Malica, Eric Macke, Marnik Bercx, Sebastian P. Huber, Iurii Timrov, Nicola Marzari, First-principles Hubbard parameters with automated and reproducible workflows, Materials Cloud Archive 2025.33 (2025), https://doi.org/10.24435/materialscloud:v2-60

Description

We introduce an automated, flexible framework (aiida-hubbard) to self-consistently calculate Hubbard U and V parameters from first-principles. By leveraging density-functional perturbation theory, the computation of the Hubbard parameters is efficiently parallelized using multiple concurrent and inexpensive primitive cell calculations. Furthermore, the intersite V parameters are defined on-the-fly during the iterative procedure to account for atomic relaxations and diverse coordination environments. We devise a novel, code-agnostic data structure to store Hubbard related information together with the atomistic structure, to enhance the reproducibility of Hubbard-corrected calculations. We demonstrate the scalability and reliability of the framework by computing in high-throughput fashion the self-consistent onsite U and intersite V parameters for 115 Li-containing bulk solids with up to 32 atoms in the unit cell. Our analysis of the Hubbard parameters calculated reveals a significant correlation of the onsite U values on the oxidation state and coordination environment of the atom on which the Hubbard manifold is centered, while intersite V values exhibit a general decay with increasing interatomic distance. We find, e.g., that the numerical values of U for the 3d orbitals of Fe and Mn can vary up to 3 eV and 6 eV, respectively; their distribution is characterized by typical shifts of about 0.5 eV and 1.0 eV upon change in oxidation state, or local coordination environment. For the intersite V a narrower spread is found, with values ranging between 0.2 eV and 1.6 eV when considering transition metal and oxygen interactions. This framework paves the way for the exploration of redox materials chemistry and high-throughput screening of d and f compounds across diverse research areas, including the discovery and design of novel energy storage materials, as well as other technologically-relevant applications.

Materials Cloud sections using this data

Files

File name	Size	Description
README.md MD5md5:bb2551e4d69825a996c3144205ae9f8e	3.2 KiB	Instructions on how to reproduce the calculations and navigate the AiiDA repository.
scripts.tar.gz MD5md5:cb4f697364df39852ee2f4eec9640df1	88.3 KiB	Tarball containing the scripts used to run the high-throughput calculations, as well as jupyter notebooks used to produce the main figures and tables of the study.
archive.aiida MD5md5:8f16db128d01222efe383031e64b5882 Open this AiiDA archive on renkulab.io (https://renkulab.io/)	248.4 MiB	AiiDA database containing the self-consistent results of the Hubbard parameters for 105 Li-containing TM (TM=Fe, Mn) compounds. Note that the first step of the self-consistent cycle has been removed from the provenance due to licensing constraints (the initial structures were taken from experimental databases).

License

Files and data are licensed under the terms of the following license: Creative Commons Attribution 4.0 International.
Metadata, except for email addresses, are licensed under the Creative Commons Attribution Share-Alike 4.0 International license.

External references

Keywords

Oxidation state DFT+U+V DFT+U Hubbard AiiDA