Excited-state hyper-Rayleigh scattering measurements of organic molecules

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Optical enhancement or decrease of the nonlinear optical (NLO) properties of organic compounds is expected at the excited state due to changes in dipole moments and oscillator strength caused by electron density distribution different from that at the ground state. It is necessary to evaluate NLO properties at the excited state in development and practical application of highly functional organic molecules. A novel excited state hyper-Rayleigh scattering (HRS) measurement system was constructed to evaluate hyperpolarizability (beta) at the excited state of molecules in solutions. The system is composed of a ns Nd:YAG probe laser of various intensities and a ns tunable pump laser for excitation. The HRS intensity at 2(omega) for p-nitoaniline in methanol solutions, proportional to the square of the incident laser power, increased upon excitation at 464nm and also depended on the delay time between a pump and a probe pulse. The (beta) value for p-nitroaniline at the excited triplet state was evaluated.

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