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Title: 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 nanosys- tems 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. In this work 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. Moreover, when applied to the Kretschmann configu- ration, we show that the excitation of propagating plasmons leads to a broader energy distribution of electrons due to the enhanced Landau damping.
Authors:
 [1] ;  [2] ;  [3] ;  [1] ;  [1] ;  [2]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Emory Univ., Atlanta, GA (United States)
  3. Ohio Univ., Athens, OH (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1461506

Heilpern, Tal, Manjare, Manoj, Govorov, Alexander O., Wiederrecht, Gary P., Gray, Stephen K., and Harutyunyan, Hayk. Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements. United States: N. p., Web. doi:10.1038/s41467-018-04289-3.
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. United States. doi:10.1038/s41467-018-04289-3.
Heilpern, Tal, Manjare, Manoj, Govorov, Alexander O., Wiederrecht, Gary P., Gray, Stephen K., and Harutyunyan, Hayk. 2018. "Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements". United States. doi:10.1038/s41467-018-04289-3. https://www.osti.gov/servlets/purl/1461506.
@article{osti_1461506,
title = {Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements},
author = {Heilpern, Tal and Manjare, Manoj and Govorov, Alexander O. and Wiederrecht, Gary P. and Gray, Stephen K. and Harutyunyan, Hayk},
abstractNote = {Developing a fundamental understanding of ultrafast non-thermal processes in metallic nanosys- tems 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. In this work 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. Moreover, when applied to the Kretschmann configu- ration, we show that the excitation of propagating plasmons leads to a broader energy distribution of electrons due to the enhanced Landau damping.},
doi = {10.1038/s41467-018-04289-3},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {5}
}

Works referenced in this record:

Optical Constants of the Noble Metals
journal, December 1972