Nonlinear optical and light emission studies of special organic molecules and crystals

The nonlinear optical properties and light emission characteristics of some special organic molecules and crystals have been studied in detail. The second-order nonlinear optical effects were measured in the single-crystal films of the materials. The crystallographic orientations of the films were determined using x-ray diffraction measurements. The second-order susceptibility tensor elements of 4-aminobenzophenone (ABP) and 8-(4'-acetylphenyl)-1,4-dioxa-8-azaspiro[4.5]decane (APDA) films were measured using polarization selective second-harmonic generation experiments. The d-coefficients of ABP are: d 23 = 7.3 +/- 0.4 pm/V and d22 = 0.73 +/- 0.04 pm/V, while those of APDA are: d33 = 54 +/- 6 pm/V and d15 = 18 +/- 3 pm/V at 1064 nm. Phase-matched propagation directions were identified on the films. The application of these films in measuring ultra-short laser pulse-width was demonstrated. Polarized optical absorption and photo-luminescence were measured in 4'-dimethylamino-N-methyl-4-stilbazolium tosylate (DAST). The electro-optic properties of single-crystal films of DAST and styryl pyridinium cyanine dye (SPCD) were studied over a broad range of wavelengths. The measured r-coefficients are the largest reported in any material. Thin-film electro-optic modulators were demonstrated using these films which have insignificant insertion and propagation losses compared to the traditional waveguide based devices. The response was observed to be flat over the measured frequency range (2 kHz--100 MHz), which indicates the origin of the electro-optic effect to be predominantly electronic. Thus these materials have significant potential for applications in high-speed optical signal processing. Spectral broadening of femtosecond laser pulses in poly-[2,4 hexadiyne-1,6 diol-bis-(p-toluene sulfonate)] (PTS) single-crystals due to self-phase modulation was studied. The magnitudes of the nonlinear refractive index were determined over the wavelength range of 720--1064 nm. The two-photon absorption spectrum, determined from nonlinear transmission measurements, was observed to have no discernible influence on the dispersion of the nonlinear index at these wavelengths. Highly efficient spectrally narrowed emission has been observed for the first time in strongly dipolar organic salts based on the stilbazolium chromophore. An unusually high conversion efficiency (40%) with a low excitation threshold (<1 muJ) has been observed despite a very low photoluminescence efficiency (∼0.3%). The results are explained in terms of cooperative emission upon short-pulse optical excitation. These materials have a wide range of potential applications in photonics, including frequency conversion, high-speed electro-optic modulation, sensors, and novel laser-like light sources.