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Electronic structure and dynamical correlations in antiferromagnetic ${BiFeO}_{3}$

Yihan Wu ^1,2,*, Mario Caserta ^1,*, Tommaso Chiarotti ³, and Nicola Marzari ^1,4,5,†

¹Theory and Simulation of Materials (THEOS) and National Center for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland
²Institute of Physics, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland
³Department of Applied Physics and Materials Science, California Institute of Technology, Pasadena, California 91125, USA
⁴PSI Center for Scientific Computing, Theory and Data, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
⁵Theory of Condensed Matter, Cavendish Laboratory, University of Cambridge, Cambridge CB3 0US, United Kingdom

^*These authors contributed equally to this work.
^†Contact author: nicola.marzari@epfl.ch

Phys. Rev. Research 8, 033375 – Published 29 September, 2026

DOI: https://doi.org/10.1103/stw8-9mld

Abstract

We study the electronic structure and dynamical correlations in antiferromagnetic ${BiFeO}_{3}$ , a prototypical room-temperature multiferroic, using a variety of static and dynamical first-principles methods. Conventional static Hubbard corrections ( $DFT + U, DFT + U + V$ ) incorrectly predict a deep-valence Fe $3 d$ peak (around $- 7 eV$ ) in antiferromagnetic ${BiFeO}_{3}$ , in contradiction with hard x-ray photoemission. We resolve this failure by using a recent generalization of $DFT + U$ to include a frequency-dependent screening— $DFT + U (ω)$ —or using a dynamical Hubbard functional. The screened Coulomb interaction $U (ω)$ , computed with spin-polarized random-phase approximation and projected onto maximally localized Fe $3 d$ Wannier orbitals, is expressed as a sum over poles, yielding a self-energy that augments the Kohn-Sham Hamiltonian. This $DFT + U (ω)$ approach predicts a fundamental band gap of $1.53 eV$ , consistent with experiments, and completely eliminates the unphysical deep-valence peak. The resulting simulated hard x-ray photoelectron spectroscopy spectrum reproduces the experimental line shape with an accuracy comparable to state-of-the-art approaches. Our work highlights the critical nature of dynamical screening in complex oxides and of $DFT + U (ω)$ as a predictive and computationally efficient approach to address the electronic structure of correlated materials.

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Phys. Rev. Research 8, 033375– Published 29 September, 2026

Vol. 8, Iss. 3 — September - November 2026

Received 11 February 2026
Accepted 11 August 2026

DOI: https://doi.org/10.1103/stw8-9mld

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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Electronic structure and dynamical correlations in antiferromagnetic ${BiFeO}_{3}$

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Electronic structure and dynamical correlations in antiferromagnetic BiFeO3

Abstract

Physics Subject Headings (PhySH)

Article Text

References (42)

Electronic structure and dynamical correlations in antiferromagnetic ${BiFeO}_{3}$