Eric Macke^1*, Iurii Timrov^2,3*, Nicola Marzari^2,4*, Lucio Colombi Ciacchi^1*

1 Faculty of Production Engineering, Bremen Center for Computational Materials Science and MAPEX Center for Materials and Processes, Hybrid Materials Interfaces Group, University of Bremen, Am Fallturm 1, 28359 Bremen, Germany

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

3 Present address: Laboratory for Materials Simulations (LMS), Paul Scherrer Institut (PSI), CH-5232 Villigen PSI, Switzerland

4 University of Bremen Excellence Chair, Bremen Center for Computational Materials Science, University of Bremen, Bibliothekstraße 1, 28359 Bremen, Germany

* Corresponding authors emails: emacke@uni-bremen.de, iurii.timrov@psi.ch, nicola.marzari@epfl.ch, colombi@hmi.uni-bremen.de

DOI10.24435/materialscloud:tw-b5 [version v1]

Publication date: Apr 08, 2024

How to cite this record

Eric Macke, Iurii Timrov, Nicola Marzari, Lucio Colombi Ciacchi, Orbital-resolved DFT+U for molecules and solids, Materials Cloud Archive 2024.53 (2024), https://doi.org/10.24435/materialscloud:tw-b5

Description

We present an orbital-resolved extension of the Hubbard U correction to density-functional theory (DFT). Compared to the conventional shell-averaged approach, the prediction of energetic, electronic and structural properties is strongly improved, particularly for compounds characterized by both localized and hybridized states in the Hubbard manifold. The numerical values of all Hubbard parameters are readily obtained from linear-response calculations. The relevance of this more refined approach is showcased by its application to bulk solids pyrite (FeS₂) and pyrolusite (β-MnO₂), as well as to six Fe(II) molecular complexes. Our findings indicate that a careful definition of Hubbard manifolds is indispensable for extending the applicability of DFT+U beyond its current boundaries. The present orbital-resolved scheme aims to provide a computationally undemanding yet accurate tool for electronic structure calculations of charge-transfer insulators, transition-metal (TM) complexes and other compounds displaying significant orbital hybridization. This dataset contains all Quantum ESPRESSO input and output files as well as all pseudopotentials that were used to generate the results of this study. Moreover, an ``EXAMPLES'' folder provides guidance on how to apply the LR-cDFT approach to evaluate orbital-resolved DFT+U parameters in practise.

Materials Cloud sections using this data

Files

File name	Size	Description
arxiv_2312.13580_RAWDATA.zip MD5md5:fcdfc1abf15fa0923695a900e5724a23	79.1 MiB	Quantum ESPRESSO input and output files used to generate the results of the study.
README.txt MD5md5:aca2d46d1613725f7cc067867bf017f7	12.3 KiB	README file explaining the data structure and also providing a brief introduction to practical evaluations of orbital-resolved Hubbard U parameters.

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

DFT+U Hubbard orbital-resolved DFT+U+V Quantum ESPRESSO LR-cDFT cDFT DFT linear response constrained DFT MARVEL