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Single-particle absorption spectroscopy by photothermal contrast.

Mustafa Yorulmaz1, Sara Nizzero1, Anneli Hoggard1

  • 1†Department of Chemistry, ‡Applied Physics Graduate Program, §Department of Electrical and Computer Engineering, Laboratory for Nanophotonics, Rice University, Houston, Texas 77005, United States.

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Summary

This study introduces a new method for pure absorption spectroscopy on single nanoparticles. It reveals unique spectral shifts between absorption and scattering in gold nanostructures, advancing nanoscale optical measurements.

Keywords:
Single-particle spectroscopyabsorption spectroscopygold nanoparticlegold nanorodphotothermal imagingsurface plasmon

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Area of Science:

  • Nanophotonics and Spectroscopy
  • Materials Science
  • Plasmonics

Background:

  • Single-particle spectroscopy advances fields by removing sample heterogeneity effects.
  • While background-free luminescence and scattering spectroscopy are common, pure absorption spectroscopy of individual nanostructures remains challenging.
  • Extinction measurements typically combine absorption and scattering, obscuring pure absorption features.

Purpose of the Study:

  • To develop and demonstrate a method for recording pure absorption spectra of individual nanostructures.
  • To investigate the spectral differences between absorption and scattering in plasmonic nanoparticles.
  • To analyze the relationship between nanorod aspect ratio and the spectral shift between absorption and scattering.

Main Methods:

  • Implementation of single-particle absorption spectroscopy using photothermal microscopy.
  • Combination with a supercontinuum laser and an advanced calibration procedure.
  • Accounting for chromatic aberrations and wavelength-dependent excitation power.

Main Results:

  • Successful recording of pure absorption spectra from individual gold nanoparticles.
  • Observed blueshift of absorption spectra compared to scattering spectra, consistent with Mie theory.
  • Demonstrated the ability to record absorption spectra across a 300 nm wavelength range for gold nanorods of varying aspect ratios.
  • Found that the spectral shift between absorption and scattering for longitudinal plasmon resonance decreases with increasing nanorod aspect ratio.

Conclusions:

  • The developed method enables pure absorption spectroscopy on individual nanostructures, overcoming limitations of extinction measurements.
  • The study confirms theoretical predictions regarding spectral shifts and provides new insights into plasmonic behavior.
  • Results offer a valuable tool for characterizing nanoscale optical properties and understanding structure-property relationships in nanomaterials.