We have increased the precision of frequency-resolved hyper-Rayleigh scattering by measuring the full Fourier transform of the time-dependent hyper-Rayleigh scattering signal. We show that adding the measurement of the phase shift between the immediate hyper-Rayleigh scattering and time-delayed fluorescence to the measurement of the demodulation of the fluorescence increases the precision of the setup with up to one order of magnitude. We have used this increased precision to determine the impact of f-orbital filling on the first hyperpolarizability of four lanthanate complexes containing the hemicyanine 1 -hexadecyl-4- {2- [4- (dimethylamino)phenyl] ethenyl} pyridinium chromophore. A detailed analysis of the fitting equations is also given.

© 2001 Optical Society of America

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