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A detailed comparison is given of several theoretical expressions commonly used in the determination of the molecular orientation in monolayers by reflection second-harmonic-generation measurements. The experimental data obtained from the Langmuir films of a hemicyanine dye are used to demonstrate that the deduced molecular-orientation angle depends sensitively on the linear dielectric constants of the monolayer. It is also pointed out that an unambiguous determination of the nonlinear susceptibilities of a monolayer by reflection second-harmonic generation requires measurements that use at least three different polarization combinations.
Zhang et al. (Fri,) studied this question.