Effective polarizabilities and local field corrections for nonlinear optical experiments in condensed media

A consistent extension of Onsager’s reaction field model to nonlinear-optical experiments in condensed media is presented. This model is used to derive effective (nonresonant) linear and nonlinear molecular polarizabilities involved in refractive index measurements, electric-field induced second-har...

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Bibliographic Details
Published in:The Journal of chemical physics 1998-01, Vol.108 (3), p.1001-1007
Main Authors: Wortmann, Rüdiger, Bishop, David M.
Format: Article
Language:English
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Summary:A consistent extension of Onsager’s reaction field model to nonlinear-optical experiments in condensed media is presented. This model is used to derive effective (nonresonant) linear and nonlinear molecular polarizabilities involved in refractive index measurements, electric-field induced second-harmonic generation, hyper-Rayleigh scattering, third-harmonic generation and degenerate four-wave mixing. The commonly applied Lorentz correction, while being a useful approximation in linear optics, is demonstrated to lead to systematic errors of typically 20% in nonlinear optical experiments. This is due to an inherent inconsistency that originates from the implicit assumption of a cavity field factor for the nonlinear molecular response.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.475462