Parthasarathy, Venkatakrishnan and Pandey, Ravindra and Das, Puspendu Kumar and Castet, Frederic and Blanchard-Desce, Mireille (2018) Linear and Nonlinear Optical Properties of Tricyanopropylidene-Based Merocyanine Dyes: Synergistic Experimental and Theoretical Investigations. In: CHEMPHYSCHEM, 19 (2). pp. 187-197.
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New merocyanines dyes with tricyanopropylidene-based acceptor units connected to dihexylaminophenyl or dihexylaminothiophenyl donor moieties through polyenic bridges of different lengths have been designed. All derivatives exhibited a strong dipolar character and showed a typical intramolecular charge transfer (ICT) transition. NMR spectroscopy experiments combined with DFT calculations demonstrated that both the nature of the donor-acceptor pair and the length of the conjugated linker strongly impact the electronic structure of the dyes and induce alteration in the bond-length alternation (BLA) and marked shifts in the ICT absorption bands. Hyper-Rayleigh scattering experiments revealed an exponential increase in the second-harmonic generation response as the polyenic chain length was increased. Strikingly, the largest chromophores with the strongest donor-acceptor pair exhibited a very high first hyperpolarizabilty together with a cyanine-like electronic structure, which apparently contradicts the paradigm of optimal BLA predicted by the two-state model. Although it decreased as the polyenic chain length increased, all dyes also exhibited high thermal stability, which demonstrates their potential for applications in nonlinear optical devices.
| Item Type: | Journal Article |
|---|---|
| Publication: | CHEMPHYSCHEM |
| Additional Information: | Copy right for this article belong to the WILEY-V C H VERLAG GMBH, POSTFACH 101161, 69451 WEINHEIM, GERMANY |
| Department/Centre: | Division of Chemical Sciences > Inorganic & Physical Chemistry |
| Date Deposited: | 02 Mar 2018 15:05 |
| Last Modified: | 02 Mar 2018 15:05 |
| URI: | http://eprints.iisc.ac.in/id/eprint/58910 |
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