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Sum frequency generation as a proxy for ellipsometry: Not just a phase.

Thorn A Dramstad¹, Zhihao Wu¹, Aaron M Massari¹

¹University of Minnesota-Twin Cities, 207 Pleasant St. SE, Minneapolis, Minnesota 55454, USA.

The Journal of Chemical Physics

|March 23, 2022

Summary

This summary is machine-generated.

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This study introduces a new method for analyzing vibrational sum frequency generation (VSFG) spectroscopy. It allows simultaneous determination of interfacial molecular responses and infrared refractive indices for organic thin films.

Area of Science:

Spectroscopy
Materials Science
Physical Chemistry

Background:

Infrared refractive indices of organic materials are typically determined using infrared (IR) ellipsometry.
Optical interference effects are crucial for solving optical constants but complicate coherent spectroscopy analysis on thin films.
Vibrational sum frequency generation (VSFG) is an interface-specific coherent spectroscopy requiring spectral modeling for accurate analysis.

Purpose of the Study:

To explore a novel approach for simultaneously obtaining molecular responses and refractive indices in VSFG experiments.
To leverage incident beam geometries and sample thicknesses for enhanced data analysis.
To improve the fidelity of fitted parameters by globally fitting multiple spectra.

Main Methods:

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Utilizing VSFG spectroscopy with varied incident beam geometries and sample thicknesses.

Developing a spectral modeling approach to account for optical interference.

Globally fitting multiple VSFG spectra using a single set of refractive indices.

Comparing results with traditional IR ellipsometry.

Main Results:

Demonstrated the feasibility of simultaneously extracting molecular responses and refractive indices.
Showcased that global fitting of multiple spectra enhances parameter fidelity.
Validated the method across organic samples of varying thicknesses.
Achieved comparable results to established IR ellipsometry techniques.

Conclusions:

The proposed method offers a powerful alternative for characterizing organic thin films.
Simultaneous determination of optical constants and molecular information simplifies VSFG data analysis.
This approach enhances the understanding of interfacial molecular dynamics and optical properties.