Thermodynamic stabilization and electronic effects of oxygen vacancies at BiFeO$_3$ neutral ferroelectric domain walls

Fuente: arXiv
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Main Authors: Zhao, Guo-Dong, Dabo, Ismaila, Chen, Long-Qing
Format: Preprint
Published: 2025
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author Zhao, Guo-Dong
Dabo, Ismaila
Chen, Long-Qing
author_facet Zhao, Guo-Dong
Dabo, Ismaila
Chen, Long-Qing
contents Enhanced conductivity at ferroelectric domain walls in BiFeO$_3$ has been widely observed, yet the microscopic origins of this effect, including electronic contributions from domain-wall defects, are incompletely understood at the atomistic level. Here, we carry out first-principles simulations to quantify the thermodynamic stability and electronic impact of oxygen vacancies at charge-neutral 71$^\circ$, 109$^\circ$, and 180$^\circ$ domain walls of BiFeO$_3$. We find that vacancies are energetically favored at domain walls by up to 0.3 eV compared to the bulk, leading to orders-of-magnitude increase in vacancy equilibrium concentration. The corresponding formation energy landscapes are discontinued and explained by local bond weakening. The vacancies induce localized electronic intragap states corresponding to small polarons, which promote thermally activated n-type conduction in the low-current regime, and their tendency to aggregate facilitate Schottky emission in the high-current regime. Our results provide a quantitative foundation for interpreting domain-wall conduction, offer guidance for defect engineering in ferroelectrics, and provide important information to phase-field simulations of defect-domain wall interactions in a ferroelectric domain structure.
format Preprint
id arxiv_https___arxiv_org_abs_2507_11863
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Thermodynamic stabilization and electronic effects of oxygen vacancies at BiFeO$_3$ neutral ferroelectric domain walls
Zhao, Guo-Dong
Dabo, Ismaila
Chen, Long-Qing
Materials Science
Enhanced conductivity at ferroelectric domain walls in BiFeO$_3$ has been widely observed, yet the microscopic origins of this effect, including electronic contributions from domain-wall defects, are incompletely understood at the atomistic level. Here, we carry out first-principles simulations to quantify the thermodynamic stability and electronic impact of oxygen vacancies at charge-neutral 71$^\circ$, 109$^\circ$, and 180$^\circ$ domain walls of BiFeO$_3$. We find that vacancies are energetically favored at domain walls by up to 0.3 eV compared to the bulk, leading to orders-of-magnitude increase in vacancy equilibrium concentration. The corresponding formation energy landscapes are discontinued and explained by local bond weakening. The vacancies induce localized electronic intragap states corresponding to small polarons, which promote thermally activated n-type conduction in the low-current regime, and their tendency to aggregate facilitate Schottky emission in the high-current regime. Our results provide a quantitative foundation for interpreting domain-wall conduction, offer guidance for defect engineering in ferroelectrics, and provide important information to phase-field simulations of defect-domain wall interactions in a ferroelectric domain structure.
title Thermodynamic stabilization and electronic effects of oxygen vacancies at BiFeO$_3$ neutral ferroelectric domain walls
topic Materials Science
url https://arxiv.org/abs/2507.11863