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• W2890598281 abstract "Multipolar chromophores (e.g., quadrupolar and octupolar molecules) have excellent two-photon absorption properties and exhibit characteristic excited-state relaxation behaviors that involve structural symmetry breaking. Environmental rigidity could provide an appreciable impact on such conformational rearrangement in the excited state; however, details of its effect remain unclear. Herein, we undertake an ensemble and single-molecule spectroscopic investigation into the effects of environmental rigidity on the photophysical characteristics and behaviors of a newly synthesized D−π–A−π–D (donor−π–acceptor−π–donor) quadrupolar chromophore, QC, and its π–A−π analogue, AC, in various solutions and polymers. The fluorescence emission of QC in nonpolar solvents takes place in the symmetric quadrupolar state [Dδ+–π–Aδ−–π–Dδ+]*, whereas the significant fluorescence quenching is observed with increasing solvent polarity, suggesting the gradual stabilization of the nonemissive symmetry-broken dipolar state [Dδ+–π–Aδ−]*−π–D or D−π–[Aδ−–π–Dδ+]* in more polar solvents. However, because of a lack of environmental rearrangement, this dipolar state is not effectively stabilized in a polar polymer matrix. Single-molecule fluorescence spectroscopy was used to explore how environmental rigidity affects the photophysical behaviors of QC and AC. In a rubbery poly(methyl acrylate) (PMA) film, the QC and AC single molecules exhibited fluorescence properties similar to those in nonpolar solutions. Remarkably, the average fluorescence lifetime of QC in the glassy PMA film was longer than that in the rubbery film. Moreover, the heterogeneity of single-molecule fluorescence lifetimes increased considerably, although such variation was not observed for the nonquadrupolar chromophore AC. Experimental and theoretical considerations suggest that fluorescence emission of QC embedded in the rubbery polymer most probably occurs from the symmetric quadrupolar state formed through planarization, whereas such conformational relaxation is suppressed in the glassy polymer because the physical constraint and various degree-of-twist conformations of QC emit fluorescence photons. Overall, this study reveals that environmental rigidity appreciably alters the photophysical characteristics and behaviors of quadrupolar chromophores." @default.
• W2890598281 created "2018-09-27" @default.
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• W2890598281 date "2018-09-03" @default.
• W2890598281 modified "2023-10-18" @default.
• W2890598281 title "Impacts of Environmental Rigidity on Photophysical Characteristics and Behaviors of a Quadrupolar Chromophore Revealed by Single-Molecule Fluorescence Spectroscopic Study" @default.
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• W2890598281 doi "https://doi.org/10.1021/acs.jpcc.8b03889" @default.
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