Direct, indirect, and self-trapped excitons in Cs$_2$AgBiBr$_6$

Fuente: arXiv
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Autori principali: Baskurt, Mehmet, Erhart, Paul, Wiktor, Julia
Natura: Preprint
Pubblicazione: 2024
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author Baskurt, Mehmet
Erhart, Paul
Wiktor, Julia
author_facet Baskurt, Mehmet
Erhart, Paul
Wiktor, Julia
contents Cs$_2$AgBiBr$_6$ exhibits promising photovoltaic and light-emitting properties, making it a candidate for next-generation solar cells and LED technologies. Additionally, it serves as a model system within the family of halide double perovskites, offering insights into the broader class of materials. Here, we study various possible excited states of this material to understand its absorption and emission properties. We use Time-Dependent Density Functional Theory (TD-DFT) coupled with non-empirical hybrid functionals, specifically PBE0($α$) and dielectric-dependent hybrids (DDH) to explore direct, indirect, and self-trapped excitons in this material. Based on comparison with experiment, we show that these methods can give excellent prediction of the absorption spectrum and that the fundamental band gap has been underestimated in previous computational studies. We connect the experimental photoluminescence signals at 1.9-2.0 eV to the emission from self-trapped excitons and electron polarons. Finally, we reveal a complex landscape with energetically competing direct, indirect, and self-trapped excitons in the material.
format Preprint
id arxiv_https___arxiv_org_abs_2405_20017
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Direct, indirect, and self-trapped excitons in Cs$_2$AgBiBr$_6$
Baskurt, Mehmet
Erhart, Paul
Wiktor, Julia
Materials Science
Cs$_2$AgBiBr$_6$ exhibits promising photovoltaic and light-emitting properties, making it a candidate for next-generation solar cells and LED technologies. Additionally, it serves as a model system within the family of halide double perovskites, offering insights into the broader class of materials. Here, we study various possible excited states of this material to understand its absorption and emission properties. We use Time-Dependent Density Functional Theory (TD-DFT) coupled with non-empirical hybrid functionals, specifically PBE0($α$) and dielectric-dependent hybrids (DDH) to explore direct, indirect, and self-trapped excitons in this material. Based on comparison with experiment, we show that these methods can give excellent prediction of the absorption spectrum and that the fundamental band gap has been underestimated in previous computational studies. We connect the experimental photoluminescence signals at 1.9-2.0 eV to the emission from self-trapped excitons and electron polarons. Finally, we reveal a complex landscape with energetically competing direct, indirect, and self-trapped excitons in the material.
title Direct, indirect, and self-trapped excitons in Cs$_2$AgBiBr$_6$
topic Materials Science
url https://arxiv.org/abs/2405.20017