Repository logo

Infoscience

  • English
  • French
Log In
Logo EPFL, École polytechnique fédérale de Lausanne

Infoscience

  • English
  • French
Log In
  1. Home
  2. Academic and Research Output
  3. Journal articles
  4. Understanding the role of Hubbard corrections in the rhombohedral phase of BaTiO3
 
research article

Understanding the role of Hubbard corrections in the rhombohedral phase of BaTiO3

Gebreyesus, G.
•
Bastonero, Lorenzo
•
Kotiuga, Michele  
Show more
December 27, 2023
Physical Review B

We present a first-principles study of the low-temperature rhombohedral phase of BaTiO3 using Hubbardcorrected density-functional theory. By employing density-functional perturbation theory, we compute the onsite Hubbard U for Ti(3d) states and the intersite Hubbard V between Ti(3d) and O(2p) states. We show that applying the onsite Hubbard U correction alone to Ti(3d) states proves detrimental, as it suppresses the Ti(3d)-O(2p) hybridization and drives the system towards a cubic phase. Conversely, when both onsite U and intersite V are considered, the localized character of the Ti(3d) states is maintained, while also preserving the Ti(3d)-O(2p) hybridization, restoring the rhombohedral phase of BaTiO3. The generalized PBEsol+U+V functional yields good agreement with experimental results for the band gap and dielectric constant, while the optimized geometry is slightly less accurate compared to PBEsol. Zone-center phonon frequencies and Raman spectra are found to be significantly influenced by the underlying geometry. PBEsol and PBEsol+U+V provide satisfactory agreement with the experimental Raman spectrum when the PBEsol geometry is used, while PBEsol+U Raman spectrum diverges strongly from experimental data highlighting the adverse impact of the U correction alone in BaTiO3. Our findings underscore the promise of the extended Hubbard PBEsol+U+V functional with first-principles U and V for the investigation of other ferroelectric perovskites with mixed ionic-covalent interactions.

  • Details
  • Metrics
Type
research article
DOI
10.1103/PhysRevB.108.235171
Web of Science ID

WOS:001144859100003

Author(s)
Gebreyesus, G.
Bastonero, Lorenzo
Kotiuga, Michele  
Marzari, Nicola  
Timrov, Iurii  
Date Issued

2023-12-27

Publisher

Amer Physical Soc

Published in
Physical Review B
Volume

108

Issue

23

Article Number

235171

Subjects

Technology

•

Physical Sciences

•

Interatomic Force-Constants

•

Born Effective Charges

•

1St-Principles Calculations

•

Barium-Titanate

•

Ferroelectricity

•

Polarization

•

Raman

•

Spectra

•

Origin

•

Stability

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
THEOS  
FunderGrant Number

tional Science Foundation

205602

Swiss National Supercomput-ing Centre (CSCS)

s1073

Centre for High Performance Computing (CHPC) , South Africa

hbc00053

Show more
Available on Infoscience
February 21, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/205099
Logo EPFL, École polytechnique fédérale de Lausanne
  • Contact
  • infoscience@epfl.ch

  • Follow us on Facebook
  • Follow us on Instagram
  • Follow us on LinkedIn
  • Follow us on X
  • Follow us on Youtube
AccessibilityLegal noticePrivacy policyCookie settingsEnd User AgreementGet helpFeedback

Infoscience is a service managed and provided by the Library and IT Services of EPFL. © EPFL, tous droits réservés