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Third harmonic scattering in liquids.

David P Shelton1

  • 1Department of Physics and Astronomy, University of Nevada, Las Vegas, Nevada 89154-4002, USA.

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|December 17, 2018
PubMed
Summary
This summary is machine-generated.

Third harmonic scattering (THS) measurements in liquids are often misinterpreted. The observed signal is primarily from coherent third harmonic generation, not direct THS, invalidating common analysis methods for pure liquids.

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Area of Science:

  • Nonlinear Optics
  • Molecular Spectroscopy
  • Physical Chemistry

Background:

  • Third harmonic scattering (THS) is a nonlinear optical phenomenon.
  • It has been proposed as a method to determine molecular second hyperpolarizability in liquids.
  • THS is considered analogous to second harmonic scattering (hyper-Rayleigh scattering).

Purpose of the Study:

  • To re-evaluate the interpretation of third harmonic scattering signals in pure liquids.
  • To investigate the contributions of coherent third harmonic generation versus direct incoherent THS.
  • To assess the validity of internal reference and polarization analysis methods for THS in pure liquids.

Main Methods:

  • Theoretical comparison of coherent third harmonic generation and direct THS processes.
  • Extensive experimental measurements on carbon tetrachloride (CCl4) liquid, silicon dioxide (SiO2) glass, and dichlorodifluoromethane (CCl2F2) gas.
  • Survey measurements on various liquids including D2O, CDCl3, CD3CN, and (CD3)2SO.

Main Results:

  • The dominant contribution to the observed THS signal in pure solvents arises from coherent third harmonic generation followed by Rayleigh scattering.
  • Direct incoherent THS constitutes a minor fraction (<2% for parallel polarized THS) of the total signal.
  • This finding invalidates the internal reference method and polarization analysis commonly applied to pure liquids.

Conclusions:

  • The interpretation of THS signals in pure liquids requires revision due to the prevalence of coherent third harmonic generation.
  • Standard analysis methods relying on direct THS are not applicable to pure liquid samples.
  • Further research is needed to develop accurate methods for determining molecular hyperpolarizability using THS.