Hyper-Rayleigh scattering (HRS), or incoherent second-harmonic generation,
from Langmuir films of C-60 and its derivatives deposited upon fused-quartz
substrates is studied experimentally. For C-60 and C-60-tetracyanoethylene
oxide derivative (C-60([CN])) films the diffuse second-harmonic signal fro
m a single Langmuir layer is at least ten times larger than that from multi
layer films. For C-60-indopane derivative (C-60([ind])) films no peculiarit
ies in the diffuse second-harmonic signal from a single layer are observed,
whereas the ratio of the intensities of specular and diffuse signals is fo
und to be proportional to the thickness of the film. HRS indicatrices are m
easured; the results yield estimates for the correlation length of fluctuat
ions of nonlinear polarization: 100 nm for C-60 and C-60([CN]) films and 30
0 nm for C-60([ind]) films. (C) 1999 Optical Society of America [S0740-3224
(99)03309-3].