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Giant Nonlinear Optical Response of Interacting One-Dimensional Frenkel Excitons in Molecular Aggregates

Roman V. MarkovInstitute of Automation and Electrometry, Siberian Branch of Russian Academy of Science, 1 Academician Koptyug Ave., 630090, Novosibirsk, RussiaA. I. PlekhanovInstitute of Automation and Electrometry, Siberian Branch of Russian Academy of Science, 1 Academician Koptyug Ave., 630090, Novosibirsk, RussiaВ. В. ШелковниковNovosibirsk Institute of Organic Chemistry, Siberian Branch of Russian Academy of Science, 9 Academician Lavrentjev Ave., 630090, Novosibirsk, RussiaJasper KnoesterInstitute for Theoretical Physics and Materials Science Center, University of Groningen, Nijenborgh 4, NL-9747 AG Groningen, The Netherlands
2000en
ABI

Abstract

Experimental results for the nonlinear optical properties of thin films of molecular J-aggregates of substituted pseudoisocyanine (PIC) are reported. These molecular aggregates were found to possess a giant third-order optical nonlinearity (|χ(3)| ≈︂ 10—5 esu). Thin films of J-aggregates of PIC iodide with several different N-alkyl substituents were obtained to study the effect of disorder on the nonlinear optical properties. The spectral features of the nonlinear optical susceptibility are analyzed within a model that includes exciton–exciton interactions.

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