Abstract

Incoherent optical second harmonic (SH) generation, or hyper-Rayleigh scattering (HRS), is used to study the structure and properties of $\mathrm{Gd}/{\mathrm{C}}_{18}{\mathrm{H}}_{36}{\mathrm{O}}_2$ multilayer Langmuir–Blodgett (LB) films. SH reflection spectra (in combination with linear absorption spectra), HRS indicatrices, thickness dependence, and wave polarization diagrams are measured for s-polarized fundamental radiation. The SH radiation is entirely diffuse but predominantly s polarized, with the maximum of the HRS indicatrix shifted by 8° relative to the specular direction, which is interpreted as being due to the contribution of a fluctuating quadrupole to the nonlinear-optical response of the films. The estimated correlation length of spatial fluctuations of the nonlinear-optical polarization in the film is ∼400 nm. These properties are associated with an islandlike structure formed by Gd ions inside LB structural units.

© 2000 Optical Society of America

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