The critical role of hot carrier cooling in optically excited structural transitions

Abstract The hot carrier cooling occurs in most photoexcitation-induced phase transitions (PIPTs), but its role has often been neglected in many theoretical simulations as well as in proposed mechanisms. Here, by including the previously ignored hot carrier cooling in real-time time-dependent densit...

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Autores principales:	Wen-Hao Liu, Jun-Wei Luo, Shu-Shen Li, Lin-Wang Wang
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2021
Materias:	Materials of engineering and construction. Mechanics of materials TA401-492 Computer software QA76.75-76.765
Acceso en línea:	https://doaj.org/article/34c51db80b724a25acd4c1e3f143d6ca
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spelling	oai:doaj.org-article:34c51db80b724a25acd4c1e3f143d6ca2021-12-02T16:17:17ZThe critical role of hot carrier cooling in optically excited structural transitions10.1038/s41524-021-00582-w2057-3960https://doaj.org/article/34c51db80b724a25acd4c1e3f143d6ca2021-07-01T00:00:00Zhttps://doi.org/10.1038/s41524-021-00582-whttps://doaj.org/toc/2057-3960Abstract The hot carrier cooling occurs in most photoexcitation-induced phase transitions (PIPTs), but its role has often been neglected in many theoretical simulations as well as in proposed mechanisms. Here, by including the previously ignored hot carrier cooling in real-time time-dependent density functional theory (rt-TDDFT) simulations, we investigated the role of hot carrier cooling in PIPTs. Taking IrTe2 as an example, we reveal that the cooling of hot electrons from the higher energy levels of spatially extended states to the lower energy levels of the localized Ir–Ir dimer antibonding states strengthens remarkably the atomic driving forces and enhances atomic kinetic energy. These two factors combine to dissolute the Ir–Ir dimers on a timescale near the limit of atomic motions, thus initiating a deterministic kinetic phase transition. We further demonstrate that the subsequent cooling induces nonradiative recombination of photoexcited electrons and holes, leading to the ultrafast recovery of the Ir–Ir dimers observed experimentally. These findings provide a complete picture of the atomic dynamics in optically excited structural phase transitions.Wen-Hao LiuJun-Wei LuoShu-Shen LiLin-Wang WangNature PortfolioarticleMaterials of engineering and construction. Mechanics of materialsTA401-492Computer softwareQA76.75-76.765ENnpj Computational Materials, Vol 7, Iss 1, Pp 1-6 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	Materials of engineering and construction. Mechanics of materials TA401-492 Computer software QA76.75-76.765
spellingShingle	Materials of engineering and construction. Mechanics of materials TA401-492 Computer software QA76.75-76.765 Wen-Hao Liu Jun-Wei Luo Shu-Shen Li Lin-Wang Wang The critical role of hot carrier cooling in optically excited structural transitions
description	Abstract The hot carrier cooling occurs in most photoexcitation-induced phase transitions (PIPTs), but its role has often been neglected in many theoretical simulations as well as in proposed mechanisms. Here, by including the previously ignored hot carrier cooling in real-time time-dependent density functional theory (rt-TDDFT) simulations, we investigated the role of hot carrier cooling in PIPTs. Taking IrTe2 as an example, we reveal that the cooling of hot electrons from the higher energy levels of spatially extended states to the lower energy levels of the localized Ir–Ir dimer antibonding states strengthens remarkably the atomic driving forces and enhances atomic kinetic energy. These two factors combine to dissolute the Ir–Ir dimers on a timescale near the limit of atomic motions, thus initiating a deterministic kinetic phase transition. We further demonstrate that the subsequent cooling induces nonradiative recombination of photoexcited electrons and holes, leading to the ultrafast recovery of the Ir–Ir dimers observed experimentally. These findings provide a complete picture of the atomic dynamics in optically excited structural phase transitions.
format	article
author	Wen-Hao Liu Jun-Wei Luo Shu-Shen Li Lin-Wang Wang
author_facet	Wen-Hao Liu Jun-Wei Luo Shu-Shen Li Lin-Wang Wang
author_sort	Wen-Hao Liu
title	The critical role of hot carrier cooling in optically excited structural transitions
title_short	The critical role of hot carrier cooling in optically excited structural transitions
title_full	The critical role of hot carrier cooling in optically excited structural transitions
title_fullStr	The critical role of hot carrier cooling in optically excited structural transitions
title_full_unstemmed	The critical role of hot carrier cooling in optically excited structural transitions
title_sort	critical role of hot carrier cooling in optically excited structural transitions
publisher	Nature Portfolio
publishDate	2021
url	https://doaj.org/article/34c51db80b724a25acd4c1e3f143d6ca
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_version_	1718384223685967872

The critical role of hot carrier cooling in optically excited structural transitions

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