SPECTRAL WIDTHS FOR ELASTIC SECOND HARMONIC SCATTERING

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1966

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Ohio State University

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When a pulsed ruby laser is brought to focus in a liquid composed of molecules which lack inversion symmetry a small amount of light whose frequency is twice that of the laser is scattered. This scattering is due to orientation fluctuations and its spectral width is governed by orientation relaxation processes. Linewidths have been measured for several liquids (they ranged from 12cm−1 for CCl4 to <1cm−1, the instrument limit) and used to compute (assuming Lorentzian shapes) the relaxation time rs. The results are compared to r1, the dielectric relaxation time and r2, the relaxation time determined from measurements of the wings of the Rayleigh line. In the Debye approximation these times are related by rn4πa3ηn(n+1) where a is the molecular radius and η the viscosity. This relation is restricted to non-structured liquids (for which rnrs, the structure time) and also may not be used to compare r1 and ra when the static molecular dipole moment μ is different from zero. In this case those elements of β*** tensor (which describes the induced dipole moment according to p=μ+α:EE+βEEE which transform as μ will relax with r1 the remainder with r3.

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Author Institution: Scientific Laboratory, Ford Motor Company

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