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Nonlinear effects in single-particle photothermal imaging.

Claire A West1, Stephen A Lee2, Jesse Shooter2

  • 1Department of Chemistry, University of Washington, Seattle, Washington 98195, USA.

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Photothermal imaging now images larger, light-scattering nanoparticles. New theory and experiments reveal nonlinear pump intensity dependence and image contraction for improved nanoparticle characterization.

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Area of Science:

  • Optics and Photonics
  • Nanotechnology
  • Spectroscopy

Background:

  • Photothermal imaging traditionally detects non-emitting molecules or small, non-scattering nanoparticles.
  • Current applications extend to larger, strongly light-scattering nanoparticle structures.
  • Existing photothermal signal interpretation requires reevaluation for these larger targets.

Purpose of the Study:

  • To theoretically analyze wavelength-resolved photothermal imaging for large particle scattering.
  • To investigate the relationship between photothermal spectra and absorption spectra.
  • To experimentally validate theoretical predictions using gold nanoparticles.

Main Methods:

  • Theoretical analysis of wavelength-resolved photothermal images in the large particle scattering regime.
  • Investigating the dependence of photothermal signals on pump intensity.
  • Experimental validation using individual gold nanoparticles of varying sizes (10, 20, 100 nm radius).

Main Results:

  • Photothermal signal exhibits a nonlinear dependence on pump intensity in the large particle regime.
  • The point spread function's full-width-at-half-maximum contracts, indicating improved spatial resolution.
  • Deviations between photothermal and absorption spectra increase with pump intensity.

Conclusions:

  • The developed theory accurately describes photothermal imaging of larger, scattering nanoparticles.
  • Findings demonstrate nonlinear pump power dependence and image contraction, validating the extended theoretical framework.
  • This work broadens the applicability of photothermal imaging and spectroscopy to more complex nanoparticle systems.