Hyper-Rayleigh scattering of azulenic donor-acceptor molecules at 1064 and1907 nm

Hyper-Rayleigh scattering (HRS) has been carried out for new azulenic donor -acceptor chromophores using near-infrared laser excitation at wavelengths of 1064 and 1907 nm. Hyperpolarizabilities obtained with the 1064 nm incide nt excitation are large compared with those obtained using the 1907 nm exci tation, due to the effects of two-photon resonance enhancements in the form er case. The HRS experiment using the 1907 nm excitation, while challenging to carry it out, gives the hyperpolarizability value closer to the intrins ic molecular hyperpolarizability. The popular two-level model that is used to predict the first hyperpolarizability of donor-acceptor charge transfer chromophores is employed to compare the measurements made on the same chrom ophores with 1064 and 1907 nm excitations. The model is found not to be abl e to correlate the results obtained at the two wavelengths. The first hyper polarizability data obtained by using the 1907 nm excitation are consistent with electric field induced second harmonic generation data obtained by us ing the same wavelength. (C) 1999 American Institute of Physics. [S0021-960 6(99)00534-6].