A generalized model for time-resolved luminescence of localized carriers and applications: Dispersive thermodynamics of localized carriers

Abstract For excited carriers or electron-hole coupling pairs (excitons) in disordered crystals, they may localize and broadly distribute within energy space first, and then experience radiative recombination and thermal transfer (i.e., non-radiative recombination via multi-phonon process) processes...

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Autores principales:	Zhicheng Su, Shijie Xu
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2017
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/f6224b9c7ceb4386807bd73585a4dd70
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spelling	oai:doaj.org-article:f6224b9c7ceb4386807bd73585a4dd702021-12-02T11:41:01ZA generalized model for time-resolved luminescence of localized carriers and applications: Dispersive thermodynamics of localized carriers10.1038/s41598-017-00065-32045-2322https://doaj.org/article/f6224b9c7ceb4386807bd73585a4dd702017-02-01T00:00:00Zhttps://doi.org/10.1038/s41598-017-00065-3https://doaj.org/toc/2045-2322Abstract For excited carriers or electron-hole coupling pairs (excitons) in disordered crystals, they may localize and broadly distribute within energy space first, and then experience radiative recombination and thermal transfer (i.e., non-radiative recombination via multi-phonon process) processes till they eventually return to their ground states. It has been known for a very long time that the time dynamics of these elementary excitations is energy dependent or dispersive. However, theoretical treatments to the problem are notoriously difficult. Here, we develop an analytical generalized model for temperature dependent time-resolved luminescence, which is capable of giving a quantitative description of dispersive carrier dynamics in a wide temperature range. The two effective luminescence and nonradiative recombination lifetimes of localized elementary excitations were mathematically derived as $${{\boldsymbol{\tau }}}_{{\boldsymbol{L}}}{\boldsymbol{=}}\frac{{{\boldsymbol{\tau }}}_{{\boldsymbol{r}}}}{{\bf{1}}{\boldsymbol{+}}\tfrac{{{\boldsymbol{\tau }}}_{{\boldsymbol{r}}}}{{{\boldsymbol{\tau }}}_{{\boldsymbol{t}}{\boldsymbol{r}}}}({\bf{1}}{\boldsymbol{-}}{{\boldsymbol{\gamma }}}_{{\boldsymbol{c}}}){{\boldsymbol{e}}}^{({\boldsymbol{E}}{\boldsymbol{-}}{{\boldsymbol{E}}}_{{\boldsymbol{a}}}){\boldsymbol{/}}{{\boldsymbol{k}}}_{{\boldsymbol{B}}}{\boldsymbol{T}}}}$$ τ L = τ r 1 + τ r τ t r ( 1 − γ c ) e ( E − E a ) / k B T and $${{\boldsymbol{\tau }}}_{{\boldsymbol{n}}{\boldsymbol{r}}}{\boldsymbol{=}}\frac{{{\boldsymbol{\tau }}}_{{\boldsymbol{t}}{\boldsymbol{r}}}}{({\bf{1}}{\boldsymbol{-}}{{\boldsymbol{\gamma }}}_{{\boldsymbol{c}}})}{{\boldsymbol{e}}}^{{\boldsymbol{-}}({\boldsymbol{E}}{\boldsymbol{-}}{{\boldsymbol{E}}}_{{\boldsymbol{a}}}){\boldsymbol{/}}{{\boldsymbol{k}}}_{{\boldsymbol{B}}}{\boldsymbol{T}}}$$ τ n r = τ t r ( 1 − γ c ) e − ( E − E a ) / k B T , respectively. The model is successfully applied to quantitatively interpret the time-resolved luminescence data of several material systems, showing its universality and accuracy.Zhicheng SuShijie XuNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 7, Iss 1, Pp 1-8 (2017)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Zhicheng Su Shijie Xu A generalized model for time-resolved luminescence of localized carriers and applications: Dispersive thermodynamics of localized carriers
description	Abstract For excited carriers or electron-hole coupling pairs (excitons) in disordered crystals, they may localize and broadly distribute within energy space first, and then experience radiative recombination and thermal transfer (i.e., non-radiative recombination via multi-phonon process) processes till they eventually return to their ground states. It has been known for a very long time that the time dynamics of these elementary excitations is energy dependent or dispersive. However, theoretical treatments to the problem are notoriously difficult. Here, we develop an analytical generalized model for temperature dependent time-resolved luminescence, which is capable of giving a quantitative description of dispersive carrier dynamics in a wide temperature range. The two effective luminescence and nonradiative recombination lifetimes of localized elementary excitations were mathematically derived as $${{\boldsymbol{\tau }}}_{{\boldsymbol{L}}}{\boldsymbol{=}}\frac{{{\boldsymbol{\tau }}}_{{\boldsymbol{r}}}}{{\bf{1}}{\boldsymbol{+}}\tfrac{{{\boldsymbol{\tau }}}_{{\boldsymbol{r}}}}{{{\boldsymbol{\tau }}}_{{\boldsymbol{t}}{\boldsymbol{r}}}}({\bf{1}}{\boldsymbol{-}}{{\boldsymbol{\gamma }}}_{{\boldsymbol{c}}}){{\boldsymbol{e}}}^{({\boldsymbol{E}}{\boldsymbol{-}}{{\boldsymbol{E}}}_{{\boldsymbol{a}}}){\boldsymbol{/}}{{\boldsymbol{k}}}_{{\boldsymbol{B}}}{\boldsymbol{T}}}}$$ τ L = τ r 1 + τ r τ t r ( 1 − γ c ) e ( E − E a ) / k B T and $${{\boldsymbol{\tau }}}_{{\boldsymbol{n}}{\boldsymbol{r}}}{\boldsymbol{=}}\frac{{{\boldsymbol{\tau }}}_{{\boldsymbol{t}}{\boldsymbol{r}}}}{({\bf{1}}{\boldsymbol{-}}{{\boldsymbol{\gamma }}}_{{\boldsymbol{c}}})}{{\boldsymbol{e}}}^{{\boldsymbol{-}}({\boldsymbol{E}}{\boldsymbol{-}}{{\boldsymbol{E}}}_{{\boldsymbol{a}}}){\boldsymbol{/}}{{\boldsymbol{k}}}_{{\boldsymbol{B}}}{\boldsymbol{T}}}$$ τ n r = τ t r ( 1 − γ c ) e − ( E − E a ) / k B T , respectively. The model is successfully applied to quantitatively interpret the time-resolved luminescence data of several material systems, showing its universality and accuracy.
format	article
author	Zhicheng Su Shijie Xu
author_facet	Zhicheng Su Shijie Xu
author_sort	Zhicheng Su
title	A generalized model for time-resolved luminescence of localized carriers and applications: Dispersive thermodynamics of localized carriers
title_short	A generalized model for time-resolved luminescence of localized carriers and applications: Dispersive thermodynamics of localized carriers
title_full	A generalized model for time-resolved luminescence of localized carriers and applications: Dispersive thermodynamics of localized carriers
title_fullStr	A generalized model for time-resolved luminescence of localized carriers and applications: Dispersive thermodynamics of localized carriers
title_full_unstemmed	A generalized model for time-resolved luminescence of localized carriers and applications: Dispersive thermodynamics of localized carriers
title_sort	generalized model for time-resolved luminescence of localized carriers and applications: dispersive thermodynamics of localized carriers
publisher	Nature Portfolio
publishDate	2017
url	https://doaj.org/article/f6224b9c7ceb4386807bd73585a4dd70
work_keys_str_mv	AT zhichengsu ageneralizedmodelfortimeresolvedluminescenceoflocalizedcarriersandapplicationsdispersivethermodynamicsoflocalizedcarriers AT shijiexu ageneralizedmodelfortimeresolvedluminescenceoflocalizedcarriersandapplicationsdispersivethermodynamicsoflocalizedcarriers AT zhichengsu generalizedmodelfortimeresolvedluminescenceoflocalizedcarriersandapplicationsdispersivethermodynamicsoflocalizedcarriers AT shijiexu generalizedmodelfortimeresolvedluminescenceoflocalizedcarriersandapplicationsdispersivethermodynamicsoflocalizedcarriers
_version_	1718395496929689600

A generalized model for time-resolved luminescence of localized carriers and applications: Dispersive thermodynamics of localized carriers

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