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Main Authors: Hassani, Hamideh, Bousquet, Eric, He, Xu, Partoens, Bart, Ghosez, Philippe
Format: Preprint
Published: 2024
Subjects:
Online Access:https://arxiv.org/abs/2411.02144
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author Hassani, Hamideh
Bousquet, Eric
He, Xu
Partoens, Bart
Ghosez, Philippe
author_facet Hassani, Hamideh
Bousquet, Eric
He, Xu
Partoens, Bart
Ghosez, Philippe
contents Polarons can naturally form in materials from the interaction of extra charge carriers with the atomic lattice. Ubiquitous, they are central to various topics and phenomena such as high-T$_c$ superconductivity, electrochromism, photovoltaics, photocatalysis or ion batteries. However, polaron formation remains poorly understood and mostly relies on few historical models such as Landau-Pekar, Frölich, Holstein or Jahn-Teller polarons. Here, from advanced first-principles calculations, we show that the formation of intriguing medium-size polarons in WO$_3$ does not fit with traditional models but instead arises from the undoing of distortive atomic motions inherent to the pristine phase, which lowers the bandgap through dynamical covalency effects. We so introduce the innovative concept of {\it anti-distortive} polaron and rationalize it from a quantum-dot model. We demonstrate that anti-distortive polarons are generic to different families of compounds and clarify how this new concept opens concrete perspectives for a better control of the polaronic state and related properties.
format Preprint
id arxiv_https___arxiv_org_abs_2411_02144
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle The anti-distortive polaron : an alternative mechanism for lattice-mediated charge trapping
Hassani, Hamideh
Bousquet, Eric
He, Xu
Partoens, Bart
Ghosez, Philippe
Materials Science
Polarons can naturally form in materials from the interaction of extra charge carriers with the atomic lattice. Ubiquitous, they are central to various topics and phenomena such as high-T$_c$ superconductivity, electrochromism, photovoltaics, photocatalysis or ion batteries. However, polaron formation remains poorly understood and mostly relies on few historical models such as Landau-Pekar, Frölich, Holstein or Jahn-Teller polarons. Here, from advanced first-principles calculations, we show that the formation of intriguing medium-size polarons in WO$_3$ does not fit with traditional models but instead arises from the undoing of distortive atomic motions inherent to the pristine phase, which lowers the bandgap through dynamical covalency effects. We so introduce the innovative concept of {\it anti-distortive} polaron and rationalize it from a quantum-dot model. We demonstrate that anti-distortive polarons are generic to different families of compounds and clarify how this new concept opens concrete perspectives for a better control of the polaronic state and related properties.
title The anti-distortive polaron : an alternative mechanism for lattice-mediated charge trapping
topic Materials Science
url https://arxiv.org/abs/2411.02144