Award Date

1-1-2000

Degree Type

Thesis

Degree Name

Master of Science (MS)

Department

Physics

First Committee Member

David Shelton

Number of Pages

80

Abstract

First hyperpolarizabilities beta of carbon tetrachloride, carbon tetrafluoride, deuterated methane, and methane have been measured by hyper-Rayleigh scattering in gas and liquid phases. The gas-phase results for the coefficient beta xyz (atomic units) are 11.0 +/- 0.9 (CC14), 5.4 +/- 0.4 (CF4), 7.0 +/- 0.6 (CD4), 7.1 +/- 0.7 (CH4). Ab initio calculations are consistent with the measured values for CCl4 and CF4. A discrepancy between theory and experiment remains for CH 4, and is likely due to higher-order vibrational effects not accounted for in calculations. While the effective, liquid-phase beta for CCl 4 is 200% higher than in the gas phase due to collective scattering modes, the liquid environment has little effect on beta for the other molecules. CD4 and CH4 liquids exhibit free-rotor behavior. Liquid-gas comparisons for CF4, CD4, and CH4 show evidence that the Lorentz local-field corrections are inadequate in nonlinear optics. Through z-scan measurements, thermal lensing and/or absorption coefficients have been obtained for six molecules.

Keywords

Hyper; Hyperpolarizabilities; Measurements; Molecules; Rayleigh; Scattering; Tetrahedral

Controlled Subject

Optics; Molecular dynamics

File Format

pdf

File Size

2447.36 KB

Degree Grantor

University of Nevada, Las Vegas

Language

English

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