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• W2762445039 startingPage "29461" @default.
• W2762445039 abstract "Channel interference plays a crucial role in understanding the physics behind multiphoton absorption processes. In this work, we study the role of channel interference and solvent effects on the two-photon absorption in aryl-substituted boron dipyrromethene (BODIPY) dyes, a class of intramolecular charge-transfer (ICT) molecules. For this purpose, we consider fourteen dyes of this class with various donor/acceptor substitutions at the para position of the phenyl ring and with or without methyl (-CH3) substitution on the BODIPY moiety. The presence of a methyl group on the BODIPY moiety affects the dihedral angle significantly, which in turn affects the one- (OPA) and two-photon absorption (TPA) properties of the molecules. Among the molecules studied, the one having the strong electron-donating dimethylamino group and no methyl substitution at the BODIPY moiety is found to have the highest TPA cross section. Our few-state model analysis shows that the large TPA activity of this molecule is due to the all positive contributions from different channel interference terms. Change in dielectric constant of the medium is found to have a profound impact on both the magnitude and sign of the channel interference terms. The magnitude of destructive channel interference gradually decreases with decreasing solvent polarity and becomes constructive in a low-polarity solvent. We also study the effect of rotating the phenyl ring with respect to the BODIPY moiety on the TPA activity. In the gas phase and in different solvents, we found that channel interference is changed from destructive to constructive on twisting the molecule. These results are explained by considering different dipole-, energy- and angle-terms appearing in the expression of a two-state model." @default.
• W2762445039 created "2017-10-20" @default.
• W2762445039 creator A5049492631 @default.
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• W2762445039 date "2017-01-01" @default.
• W2762445039 modified "2023-10-14" @default.
• W2762445039 title "Interplay of twist angle and solvents with two-photon optical channel interference in aryl-substituted BODIPY dyes" @default.
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• W2762445039 doi "https://doi.org/10.1039/c7cp05679f" @default.
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