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Non-equilibrium Microwave Plasma for Efficient High Temperature Chemistry

Non-equilibrium Microwave Plasma for Efficient High Temperature Chemistry

Published on: August 1, 2017

Gas phase hyper-Rayleigh scattering measurements.

David P Shelton¹

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

The Journal of Chemical Physics

|August 3, 2012

Summary

This summary is machine-generated.

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This study measured hyper-Rayleigh scattering for nine gases, determining molecular hyperpolarizability tensor components for four. Experimental results showed significant discrepancies with theoretical calculations, even after including vibrational effects.

Area of Science:

Molecular spectroscopy
Quantum chemistry
Nonlinear optics

Background:

Hyper-Rayleigh scattering (HRS) is a nonlinear optical technique probing molecular hyperpolarizability.
Accurate determination of molecular hyperpolarizability is crucial for understanding electronic structure and nonlinear optical properties.

Purpose of the Study:

To experimentally measure hyper-Rayleigh scattering intensities and polarization ratios for nine small molecules in the gas phase.
To determine molecular hyperpolarizability tensor components for selected molecules.
To compare experimental results with ab initio calculations and assess the impact of vibrational contributions.

Main Methods:

Gas-phase hyper-Rayleigh scattering measurements.
Analysis of scattering intensities and polarization ratios.

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Comparison with ab initio computational results, including vibrational corrections.

Main Results:

Experimental hyperpolarizability data were obtained for nine small molecules.
Complete molecular hyperpolarizability tensor components were determined for CH(4), CF(4), CCl(4), and N(2)O.
Discrepancies up to 60% were observed between experimental and theoretical values.
Vibrational contributions altered the agreement between theory and experiment differently for various molecules.

Conclusions:

Experimental HRS provides valuable data for molecular hyperpolarizability.
Current ab initio methods show significant discrepancies with experimental results for these small molecules.
The inclusion of vibrational effects has a molecule-dependent impact on the theoretical-experimental agreement.