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Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements

Developing a fundamental understanding of ultrafast non-thermal processes in metallic nanosystems will lead to applications in photodetection, photochemistry and photonic circuitry. Typically, non-thermal and thermal carrier populations in plasmonic systems are inferred either by making assumptions...

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Autores principales: Heilpern, Tal, Manjare, Manoj, Govorov, Alexander O., Wiederrecht, Gary P., Gray, Stephen K., Harutyunyan, Hayk
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5945638/
https://www.ncbi.nlm.nih.gov/pubmed/29748626
http://dx.doi.org/10.1038/s41467-018-04289-3
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author Heilpern, Tal
Manjare, Manoj
Govorov, Alexander O.
Wiederrecht, Gary P.
Gray, Stephen K.
Harutyunyan, Hayk
author_facet Heilpern, Tal
Manjare, Manoj
Govorov, Alexander O.
Wiederrecht, Gary P.
Gray, Stephen K.
Harutyunyan, Hayk
author_sort Heilpern, Tal
collection PubMed
description Developing a fundamental understanding of ultrafast non-thermal processes in metallic nanosystems will lead to applications in photodetection, photochemistry and photonic circuitry. Typically, non-thermal and thermal carrier populations in plasmonic systems are inferred either by making assumptions about the functional form of the initial energy distribution or using indirect sensors like localized plasmon frequency shifts. Here we directly determine non-thermal and thermal distributions and dynamics in thin films by applying a double inversion procedure to optical pump-probe data that relates the reflectivity changes around Fermi energy to the changes in the dielectric function and in the single-electron energy band occupancies. When applied to normal incidence measurements our method uncovers the ultrafast excitation of a non-Fermi-Dirac distribution and its subsequent thermalization dynamics. Furthermore, when applied to the Kretschmann configuration, we show that the excitation of propagating plasmons leads to a broader energy distribution of electrons due to the enhanced Landau damping.
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spelling pubmed-59456382018-05-14 Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements Heilpern, Tal Manjare, Manoj Govorov, Alexander O. Wiederrecht, Gary P. Gray, Stephen K. Harutyunyan, Hayk Nat Commun Article Developing a fundamental understanding of ultrafast non-thermal processes in metallic nanosystems will lead to applications in photodetection, photochemistry and photonic circuitry. Typically, non-thermal and thermal carrier populations in plasmonic systems are inferred either by making assumptions about the functional form of the initial energy distribution or using indirect sensors like localized plasmon frequency shifts. Here we directly determine non-thermal and thermal distributions and dynamics in thin films by applying a double inversion procedure to optical pump-probe data that relates the reflectivity changes around Fermi energy to the changes in the dielectric function and in the single-electron energy band occupancies. When applied to normal incidence measurements our method uncovers the ultrafast excitation of a non-Fermi-Dirac distribution and its subsequent thermalization dynamics. Furthermore, when applied to the Kretschmann configuration, we show that the excitation of propagating plasmons leads to a broader energy distribution of electrons due to the enhanced Landau damping. Nature Publishing Group UK 2018-05-10 /pmc/articles/PMC5945638/ /pubmed/29748626 http://dx.doi.org/10.1038/s41467-018-04289-3 Text en © The Author(s) 2018 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Heilpern, Tal
Manjare, Manoj
Govorov, Alexander O.
Wiederrecht, Gary P.
Gray, Stephen K.
Harutyunyan, Hayk
Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements
title Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements
title_full Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements
title_fullStr Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements
title_full_unstemmed Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements
title_short Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements
title_sort determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5945638/
https://www.ncbi.nlm.nih.gov/pubmed/29748626
http://dx.doi.org/10.1038/s41467-018-04289-3
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