Automated Modeling of Polarons: Defects and Reactivity on TiO$_2$(110) Surfaces

Fuente: arXiv
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Autores principales: Yalcin, Firat, Verdi, Carla, Birschitzky, Viktor C., Meier, Matthias, Wolloch, Michael, Reticcioli, Michele
Formato: Preprint
Publicado: 2025
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author Yalcin, Firat
Verdi, Carla
Birschitzky, Viktor C.
Meier, Matthias
Wolloch, Michael
Reticcioli, Michele
author_facet Yalcin, Firat
Verdi, Carla
Birschitzky, Viktor C.
Meier, Matthias
Wolloch, Michael
Reticcioli, Michele
contents Polarons are widespread in functional materials and are key to device performance in several technological applications. However, their effective impact on material behavior remains elusive, as condensed matter studies struggle to capture their intricate interplay with atomic defects in the crystal. In this work, we present an automated workflow for modeling polarons within density functional theory (DFT). Our approach enables a fully automatic identification of the most favorable polaronic configurations in the system. Machine learning techniques accelerate predictions, allowing for an efficient exploration of the defect-polaron configuration space. We apply this methodology to Nb-doped TiO$_2$(110) surfaces, providing new insights into the role of defects in surface reactivity. Using CO adsorbates as a probe, we find that Nb doping has minimal impact on reactivity, whereas oxygen vacancies contribute significantly depending on their local arrangement via the stabilization of polarons on the surface atomic layer. Our package streamlines the modeling of charge trapping and polaron localization with high efficiency, enabling systematic, large-scale investigations of polaronic effects across complex material systems.
format Preprint
id arxiv_https___arxiv_org_abs_2508_15572
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Automated Modeling of Polarons: Defects and Reactivity on TiO$_2$(110) Surfaces
Yalcin, Firat
Verdi, Carla
Birschitzky, Viktor C.
Meier, Matthias
Wolloch, Michael
Reticcioli, Michele
Materials Science
Polarons are widespread in functional materials and are key to device performance in several technological applications. However, their effective impact on material behavior remains elusive, as condensed matter studies struggle to capture their intricate interplay with atomic defects in the crystal. In this work, we present an automated workflow for modeling polarons within density functional theory (DFT). Our approach enables a fully automatic identification of the most favorable polaronic configurations in the system. Machine learning techniques accelerate predictions, allowing for an efficient exploration of the defect-polaron configuration space. We apply this methodology to Nb-doped TiO$_2$(110) surfaces, providing new insights into the role of defects in surface reactivity. Using CO adsorbates as a probe, we find that Nb doping has minimal impact on reactivity, whereas oxygen vacancies contribute significantly depending on their local arrangement via the stabilization of polarons on the surface atomic layer. Our package streamlines the modeling of charge trapping and polaron localization with high efficiency, enabling systematic, large-scale investigations of polaronic effects across complex material systems.
title Automated Modeling of Polarons: Defects and Reactivity on TiO$_2$(110) Surfaces
topic Materials Science
url https://arxiv.org/abs/2508.15572