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| - Very Large Infrared Two-Photon Absorption Cross Section of Asymmetric Zinc PorphyrinAggregates: Role of Intermolecular Interaction and Donor−Acceptor Strengths
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| - Very large two-photon absorption (TPA) cross sections at the infrared region have been revealed for J-aggregatesof asymmetric zinc porphyrin using quantum-chemical calculation. The TPA properties are evaluated formonomer and aggregates of a series of push−pull porphyrins, whose syntheses are known in the literature.The two-photon absorption cross section can be greatly enhanced by increasing the strengths of the electrondonor/acceptor. We also present a quantum-chemical analysis on porphyrin aggregates to understand the roleof intermolecular interactions and the relationship between structural and collective nonlinear optical properties.It has been observed that the TPA properties change tremendously as monomers undergo J-aggregation andthe magnitudes of TPA cross sections are highly dependent on the nature of aggregates. The importance ofour results with respect to the design of photonic and photodynamic therapy materials has been discussed.
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