Theory of the Nonlinear Optical Response in One-dimensional Systems: Charge vs. Energy Transfer

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9312029 Spano A theory for the nonlinear optical response in quasi-one- dimensional systems, such as electron-donor-acceptor crystals, halogen-bridged mixed-valence transition metal complexes, polysilanes and molecular J-aggregates will be developed in an effort to better understand the roles of energy transfer versus charge transfer in systems with varying degrees of diagonal and nondiagonal disorder. Charge and excitation delocalization affects the magnitude and size dependence of the nonlinear optical response in profoundly different ways. In the initial phases of the research, noninteracting electron and mean-field Hamiltonians will be used to obtain an analytical expression for the third order optical response. Beyond mean-field theory, numerical calculations will be conducted on finite chains and extrapolated to the crystal limit. This new grant is funded jointly by the Division of Materials Research and the Chemistry Division. %%% A theoretical research program funded jointly by the Division of Materials Research and the Chemistry Division will be initiated to calculate the nonlinear optical properties of quasi-one-dimensional materials. A thorough understanding of these materials, in the bulk limit, is necessary in order to apply them to various photonic devices. ***