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Optical and Nonlinear-Optical Properties of Pseudoisocyanine J-Aggregates with the Controlled Exciton Absorption Linewidth

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Abstract

Thin films of molecular J-aggregates of pseudoisocyanine with different linewidths of exciton absorption (from 75 to 210 cm–1) were obtained. A change in the absorption linewidth of J-aggregates was achieved by introducing organic salts into a sample. As an alternative method of varying the exciton absorption linewidth, variation in sample temperature was used. For the samples obtained, the third-order nonlinear optical susceptibility χ(3) was measured at temperatures of 80 and 293 K by the Z scan and pump–probe spectroscopy techniques and the dependence of χ(3) on the absorption linewidth W was found to follow a power law. It was revealed that the character of the function χ(3)(W) is almost independent of the method for measuring the absorption linewidth to have the form χ(3)W δ with δ ≈ –(1.36–1.58). Based on this finding, the relation of the exciton delocalization length in the aggregate to the absorption linewidth and optical nonlinearity is discussed.

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Shelkovnikov, V.V., Markov, R.V., Plekhanov, A.I. et al. Optical and Nonlinear-Optical Properties of Pseudoisocyanine J-Aggregates with the Controlled Exciton Absorption Linewidth. High Energy Chemistry 36, 260–264 (2002). https://doi.org/10.1023/A:1016277423907

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