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Orientation-insensitive methodology for second harmonic generation. 1. Theory

Simpson1, Rowlen

  • 1Department of Chemistry and Biochemistry, University of Colorado, Boulder 80309, USA.

Analytical Chemistry
|August 22, 2000
PubMed
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This study introduces a new method for measuring surface coverage using second harmonic generation. The approach minimizes errors from molecular orientation, allowing direct surface coverage determination.

Area of Science:

  • Surface Science
  • Nonlinear Optics
  • Spectroscopy

Background:

  • Second harmonic generation (SHG) is used to study surface adsorption.
  • SHG signal intensity depends on both surface coverage and molecular orientation.
  • Existing methods require complex corrections for changes in molecular orientation with coverage.

Purpose of the Study:

  • To develop a new mathematical framework for analyzing SHG intensity.
  • To identify an experimental geometry that reduces sensitivity to molecular orientation.
  • To enable direct measurement of surface coverage using SHG.

Main Methods:

  • Developed a novel mathematical model for SHG intensity as a function of excitation polarization.
  • Derived theoretical predictions for specific hyperpolarizability tensor elements (beta(z'z'z'), beta(x'x'x'), beta(x'x'z')).

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  • Identified an experimental geometry that is insensitive to molecular orientation.

    • Main Results:

    • The new approach allows for direct measurement of surface coverage.
    • Eliminates the need for tedious corrections related to molecular orientation.
    • The method is applicable to common dominant hyperpolarizability tensor elements.

    Conclusions:

    • A new SHG-based method provides direct surface coverage measurement.
    • This method overcomes limitations of traditional SHG analysis.
    • Offers a more accurate and efficient way to study adsorption processes.