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Resolving Electron-Electron Scattering in Plasmonic Nanorod Ensembles Using Two-Dimensional Electronic Spectroscopy.

William R Jeffries1, Kyoungweon Park2, Richard A Vaia2

  • 1Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States.

Nano Letters
|September 15, 2020
PubMed
Summary

Two-dimensional electronic spectroscopy (2DES) reveals electron-electron scattering dynamics in gold nanorods. This method quantifies scattering rates, offering insights into hot electron behavior in plasmonic nanoparticles.

Keywords:
Plasmonicselectron dynamicshot electronsnanoparticlestwo-dimensional electronic spectroscopy

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Spectroscopy

Background:

  • Plasmonic nanoparticles exhibit unique optical properties due to collective electron oscillations.
  • Understanding ultrafast electron dynamics is crucial for applications in catalysis, sensing, and optoelectronics.
  • Electron-electron scattering plays a significant role in the thermalization of hot electrons.

Purpose of the Study:

  • To investigate electron-electron scattering dynamics in plasmonic gold nanorods using two-dimensional electronic spectroscopy (2DES).
  • To quantify electron-electron scattering rates and their dependence on excitation conditions.
  • To demonstrate the utility of 2DES for studying hot electron dynamics in solution-phase plasmonic systems.

Main Methods:

  • Utilized two-dimensional electronic spectroscopy (2DES) to probe plasmon dephasing dynamics.
  • Monitored the time-dependent homogeneous line width (Γh(t)) of plasmons.
  • Analyzed the broadening of Γh(t) to extract electron-electron scattering rates.
  • Fitted the time-dependent Γh broadening to Fermi-liquid theory predictions.

Main Results:

  • 2DES resolved time-dependent plasmon homogeneous line width (Γh(t)), sensitive to carrier densities.
  • Excitation-induced plasmon dephasing accelerated broadening of Γh, decreasing plasmon coherence times by 20-50%.
  • Electron-electron scattering rates of ~0.01 fs-1 were obtained, increasing quadratically with excitation energy and frequency, consistent with Fermi-liquid theory.
  • Hot electron thermalization via electron-phonon scattering led to Γh narrowing.

Conclusions:

  • This study demonstrates the first application of plasmon Γh(t) to isolate electron-electron scattering dynamics in colloidal metal nanoparticles.
  • 2DES is an effective technique for studying hot electron dynamics in solution-phase plasmonic ensembles.
  • The findings provide quantitative insights into ultrafast electron scattering processes in nanomaterials.