Ab initio functional-independent calculations of the clamped Pockels tensor of tetragonal barium titanate

DOI

We present an ab initio method to calculate the clamped Pockels tensor of ferroelectric materials from density-functional theory (DFT), the modern theory of polarization exploiting the electric-enthalpy functional, and automated first- and second-order finite-difference derivatives of the polarizations and the Hellmann-Feynman forces. Thanks to the functional-independent capabilities of our approach, we can determine the Pockels tensor of tetragonal barium titanate (BTO) beyond the local density approximation (LDA), with arbitrary exchange-correlation (XC) functionals, for example, PBEsol. The latter, together with RRKJ ultra-soft pseudo-potentials (PP) and a supercell exhibiting local titanium off-centering, enables us to stabilize the negative optical phonon modes encountered in tetragonal BTO when LDA and norm-conserving PP are combined. As a result, the correct value range of r51, the largest experimental Pockels coefficient of BTO, is recovered. We also reveal that r51 increases with decreasing titanium off-centering for this material. The lessons learned from the structural, dielectric, and vibrational investigations of BTO will be essential to design next-generation electro-optical modulators based on the Pockels effect.

Identifier
DOI https://doi.org/10.24435/materialscloud:9p-tz
Related Identifier https://renkulab.io/projects/new?data=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
Related Identifier https://archive.materialscloud.org/communities/mcarchive
Related Identifier https://doi.org/10.24435/materialscloud:93-ek
Metadata Access https://archive.materialscloud.org/oai2d?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:2633
Provenance
Creator de Mestral, Virginie; Bastonero, Lorenzo; Kotiuga, Michele; Mladenovic, Marko; Marzari, Nicola; Luisier, Mathieu
Publisher Materials Cloud
Contributor de Mestral, Virginie
Publication Year 2025
Rights info:eu-repo/semantics/openAccess; Creative Commons Attribution 4.0 International; https://creativecommons.org/licenses/by/4.0/legalcode
OpenAccess true
Contact archive(at)materialscloud.org
Representation
Language English
Resource Type info:eu-repo/semantics/other
Format application/zip; text/markdown; application/octet-stream
Discipline Materials Science and Engineering