Molecular Tensor Analysis of Third-Harmonic Scattering in Liquids
| Autor: | Jack S. Ford, David L. Andrews |
|---|---|
| Rok vydání: | 2018 |
| Předmět: |
Chemistry
Scattering Isotropy Observable 02 engineering and technology 010402 general chemistry 021001 nanoscience & nanotechnology Polarization (waves) 01 natural sciences 0104 chemical sciences Quantum mechanics Homogeneous space Depolarization ratio Tensor Physical and Theoretical Chemistry 0210 nano-technology Quantum |
| Zdroj: | The Journal of Physical Chemistry A. 122:563-573 |
| ISSN: | 1520-5215 1089-5639 |
| Popis: | Third-harmonic scattering is a nonlinear optical process that involves the molecular second-hyperpolarizability, γ. This work presents a rigorous quantum electrodynamical analysis of the scattering process, involving a partially index-symmetric construction of the fourth-rank γ tensor-dispensing with the Kleinman symmetry condition. To account for stochastic molecular rotation in fluids, methods of isotropic averaging must be employed to relate the molecular properties to accessible experimental quantities such as depolarization ratio. A complete eighth-rank tensor rotational average yields results for observable third-harmonic scattering rates, cast as a function of the natural-invariant γ components, and the polarization geometry of the experiment. Decomposing the tensor γ into irreducible weights allows specific predictions to be made for each molecular point group, allowing greater discrimination between the results for different molecular symmetries. |
| Databáze: | OpenAIRE |
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