Hyper-Rayleigh scattering (HRS), or incoherent second-harmonic generation, from Langmuir films of and its derivatives deposited upon fused-quartz substrates is studied experimentally. For and -tetracyanoethylene oxide derivative films the diffuse second-harmonic signal from a single Langmuir layer is at least ten times larger than that from multilayer films. For -indopane derivative films no peculiarities in the diffuse second-harmonic signal from a single layer are observed, whereas the ratio of the intensities of specular and diffuse signals is found to be proportional to the thickness of the film. HRS indicatrices are measured; the results yield estimates for the correlation length of fluctuations of nonlinear polarization: 100 nm for and films and 300 nm for films.
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