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Influence of Electronic Non-Equilibrium on Energy Distribution and Dissipation in Aluminum Studied with an Extended Two-Temperature Model

When an ultrashort laser pulse excites a metal surface, only a few of all the free electrons absorb a photon. The resulting non-equilibrium electron energy distribution thermalizes quickly to a hot Fermi distribution. The further energy dissipation is usually described in the framework of a two-temp...

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Autores principales: Uehlein, Markus, Weber, Sebastian T., Rethfeld, Baerbel
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9145585/
https://www.ncbi.nlm.nih.gov/pubmed/35630877
http://dx.doi.org/10.3390/nano12101655
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author Uehlein, Markus
Weber, Sebastian T.
Rethfeld, Baerbel
author_facet Uehlein, Markus
Weber, Sebastian T.
Rethfeld, Baerbel
author_sort Uehlein, Markus
collection PubMed
description When an ultrashort laser pulse excites a metal surface, only a few of all the free electrons absorb a photon. The resulting non-equilibrium electron energy distribution thermalizes quickly to a hot Fermi distribution. The further energy dissipation is usually described in the framework of a two-temperature model, considering the phonons of the crystal lattice as a second subsystem. Here, we present an extension of the two-temperature model including the non-equilibrium electrons as a third subsystem. The model was proposed initially by E. Carpene and later improved by G.D. Tsibidis. We introduce further refinements, in particular, a temperature-dependent electron–electron thermalization time and an extended energy interval for the excitation function. We show results comparing the transient energy densities as well as the energy-transfer rates of the original equilibrium two-temperature description and the improved extended two-temperature model, respectively. Looking at the energy distribution of all electrons, we find good agreement in the non-equilibrium distribution of the extended two-temperature model with results from a kinetic description solving full Boltzmann collision integrals. The model provides a convenient tool to trace non-equilibrium electrons at small computational effort. As an example, we determine the dynamics of high-energy electrons observable in photo-electron spectroscopy. The comparison of the calculated spectral densities with experimental results demonstrates the necessity of considering electronic non-equilibrium distributions and electron–electron thermalization processes in time- and energy-resolved analyses.
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spelling pubmed-91455852022-05-29 Influence of Electronic Non-Equilibrium on Energy Distribution and Dissipation in Aluminum Studied with an Extended Two-Temperature Model Uehlein, Markus Weber, Sebastian T. Rethfeld, Baerbel Nanomaterials (Basel) Article When an ultrashort laser pulse excites a metal surface, only a few of all the free electrons absorb a photon. The resulting non-equilibrium electron energy distribution thermalizes quickly to a hot Fermi distribution. The further energy dissipation is usually described in the framework of a two-temperature model, considering the phonons of the crystal lattice as a second subsystem. Here, we present an extension of the two-temperature model including the non-equilibrium electrons as a third subsystem. The model was proposed initially by E. Carpene and later improved by G.D. Tsibidis. We introduce further refinements, in particular, a temperature-dependent electron–electron thermalization time and an extended energy interval for the excitation function. We show results comparing the transient energy densities as well as the energy-transfer rates of the original equilibrium two-temperature description and the improved extended two-temperature model, respectively. Looking at the energy distribution of all electrons, we find good agreement in the non-equilibrium distribution of the extended two-temperature model with results from a kinetic description solving full Boltzmann collision integrals. The model provides a convenient tool to trace non-equilibrium electrons at small computational effort. As an example, we determine the dynamics of high-energy electrons observable in photo-electron spectroscopy. The comparison of the calculated spectral densities with experimental results demonstrates the necessity of considering electronic non-equilibrium distributions and electron–electron thermalization processes in time- and energy-resolved analyses. MDPI 2022-05-12 /pmc/articles/PMC9145585/ /pubmed/35630877 http://dx.doi.org/10.3390/nano12101655 Text en © 2022 by the authors. https://creativecommons.org/licenses/by/4.0/Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Uehlein, Markus
Weber, Sebastian T.
Rethfeld, Baerbel
Influence of Electronic Non-Equilibrium on Energy Distribution and Dissipation in Aluminum Studied with an Extended Two-Temperature Model
title Influence of Electronic Non-Equilibrium on Energy Distribution and Dissipation in Aluminum Studied with an Extended Two-Temperature Model
title_full Influence of Electronic Non-Equilibrium on Energy Distribution and Dissipation in Aluminum Studied with an Extended Two-Temperature Model
title_fullStr Influence of Electronic Non-Equilibrium on Energy Distribution and Dissipation in Aluminum Studied with an Extended Two-Temperature Model
title_full_unstemmed Influence of Electronic Non-Equilibrium on Energy Distribution and Dissipation in Aluminum Studied with an Extended Two-Temperature Model
title_short Influence of Electronic Non-Equilibrium on Energy Distribution and Dissipation in Aluminum Studied with an Extended Two-Temperature Model
title_sort influence of electronic non-equilibrium on energy distribution and dissipation in aluminum studied with an extended two-temperature model
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9145585/
https://www.ncbi.nlm.nih.gov/pubmed/35630877
http://dx.doi.org/10.3390/nano12101655
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