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We performed nonlinear transmission measurements and quantum-chemical calculations on dithienothiophene (DTT)-based molecules to gain insight into the effect of acceptor and donor groups on two-photon absorption (TPA) properties. The TPA intensity showed dispersion characteristics of the single-photon absorption spectrum. When the molecules included an asymmetric donor-acceptor pair, the single- and two-photon absorption maximum wavelengths were red-shifted more than when the molecules had a symmetric donor-donor structure. We interpreted this result as indicating that the S 2 state plays the dominating role in the absorption process of molecules with a symmetric structure. The experimental TPA δ values at the absorption peak wavelength showed a dependence on the structural variations. We found the self-consistent force-field theory and Hartree-Fock Hamiltonian with single configuration interaction formalism to be valid for evaluating TPA δ. Although the quantum-chemical calculations slightly underestimated the experimental 8 values obtained from nonlinear transmission measurements, they reasonably predicted the dependence of the 8 value on the structural variations. We confirmed the role of molecular symmetry by observing that donor-donor substituted structure gave the highest experimental and theoretical TPA 8 values and that the donor-acceptor substituted structure showed a greater redshift in the TPA absorption maximum wavelength. Overall, the theoretical 8 values of DTT-based molecules were in the order of 10 -46 cm 4 .s.photon -1 and are higher than that of AF-50 by nearly two orders of magnitude.

Molecular conformations of stereoregular poly(methyl methacrylate) (PMMA) monolayers have been investigated by scanning probe microscopes. Isotactic and syndiotactic PMMAs were found to have right and left hand helical structures, respectively. On the contrary atactic PMMA showed rather random arrangement of the chains. It has been demonstrated that the PMMA Langmuir-Blodgett (LB) films can be utilized to form nanoscale patterns down to 50 nm and to form a geodesic lens. It has also been manifested that the quantum efficiency of a polymer electroluminescent device can be significantly enhanced by inserting the PMMA LB films between the emitting layer and the cathode. All the applications utilize the unique characteristics of the LB films to form thin and uniform films in the molecular level.

A blue light emitting device has been successfully fabricated using a polymer with regulated conjugation length containing trimethylsilyl substituted phenylenevinylene units. Electroluminescence from the device has an emission maximum at 470 nm. The device shows typical diode characteristics with operating voltage of 20 V and the light becomes visible at a current density of less than 0.5 mA/cm 2 . The electroluminescence spectrum is virtually identical with the photoluminescence spectrum, indicating that the radiation mechanisms are the same for both. A light emitting device using the blend of a large band gap polymer and a small band gap polymer was also fabricated. Light emission from the small band gap polymer shows much improved quantum efficiency, but there is no light emission from the large band gap polymer. Quantum efficiency of the blend increases up to about two orders of magnitude greater than that of the small band gap polymer with increasing proportion of the large band gap polymer. The improvement in quantum efficiency is interpreted in terms of exciton transfer and the hole blocking behaviour of the large band gap polymer. Finally, we have fabricated a patterned flexible light emitting device using the high quantum efficiency polymer blend system.