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Interplay of Twist Angle and Solvents With Two-Photon Optical Channel Interference in Aryl-Substituted BODIPY Dyes

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 molecules. For this purpose, we consider fourteen dyes of this class with various donor/acceptor substitutions on 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 as well as 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. The aforesaid results are explained by considering different dipole-, energy- and angle-terms appearing in the expression of a two-state model.

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Publication details

The article was received on 19 Aug 2017, accepted on 09 Oct 2017 and first published on 11 Oct 2017


Article type: Paper
DOI: 10.1039/C7CP05679F
Citation: Phys. Chem. Chem. Phys., 2017, Accepted Manuscript
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    Interplay of Twist Angle and Solvents With Two-Photon Optical Channel Interference in Aryl-Substituted BODIPY Dyes

    M. M. Alam, R. Misra and K. Ruud, Phys. Chem. Chem. Phys., 2017, Accepted Manuscript , DOI: 10.1039/C7CP05679F

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