Effective Electron Temperature Measurement Using Time-Resolved Anti-Stokes Photoluminescence

Journal Article (2020)
Author(s)

Thomas Jollans (Universiteit Leiden)

M. Caldarola (TU Delft - QN/Kuipers Lab, Kavli institute of nanoscience Delft)

Yonatan Sivan (Ben-Gurion University of the Negev)

Michel Orrit (Universiteit Leiden)

Research Group
QN/Kuipers Lab
Copyright
© 2020 Thomas Jollans, M. Caldarola, Yonatan Sivan, Michel Orrit
DOI related publication
https://doi.org/10.1021/acs.jpca.0c06671
More Info
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Publication Year
2020
Language
English
Copyright
© 2020 Thomas Jollans, M. Caldarola, Yonatan Sivan, Michel Orrit
Research Group
QN/Kuipers Lab
Issue number
34
Volume number
124
Pages (from-to)
6968-6976
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Abstract

Anti-Stokes photoluminescence of metal nanoparticles, in which emitted photons have a higher energy than the incident photons, is an indicator of the temperature prevalent within a nanoparticle. Previous work has shown how to extract the temperature from a gold nanoparticle under continuous-wave monochromatic illumination. We extend the technique to pulsed illumination and introduce pump-probe anti-Stokes spectroscopy. This new technique enables us not only to measure an effective electron temperature in a gold nanoparticle (∼103 K under our conditions), but also to measure ultrafast dynamics of a pulse-excited electron population, through its effect on the photoluminescence, with subpicosecond time resolution. We measure the heating and cooling, all within picoseconds, of the electrons and find that, with our subpicosecond pulses, the highest apparent temperature is reached 0.6 ps before the maximum change in magnitude of the extinction signal.