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The origin of the solvent dependence of fluorescence quantum yields in dipolar merocyanine dyes
Please always quote using this URN: urn:nbn:de:bvb:20-opus-198707
- Fluorophores with high quantum yields are desired for a variety of applications. Optimization of promising chromophores requires an understanding of the non-radiative decay channels that compete with the emission of photons. We synthesized a new derivative of the famous laser dye 4-dicyanomethylen-2-methyl-6-p-dimethylaminostyryl-4H-pyran (DCM),i.e., merocyanine 4-(dicyanomethylene)-2-tert-butyl-6-[3-(3-butyl-benzothiazol-2-ylidene)1-propenyl]-4H-pyran (DCBT). We measured fluorescence lifetimes and quantum yields in a variety of solventsFluorophores with high quantum yields are desired for a variety of applications. Optimization of promising chromophores requires an understanding of the non-radiative decay channels that compete with the emission of photons. We synthesized a new derivative of the famous laser dye 4-dicyanomethylen-2-methyl-6-p-dimethylaminostyryl-4H-pyran (DCM),i.e., merocyanine 4-(dicyanomethylene)-2-tert-butyl-6-[3-(3-butyl-benzothiazol-2-ylidene)1-propenyl]-4H-pyran (DCBT). We measured fluorescence lifetimes and quantum yields in a variety of solvents and found a trend opposite to the energy gap law.This motivated a theoretical investigation into the possible non-radiative decay channels. We propose that a barrier to a conical intersection exists that is very sensitive to the solvent polarity. The conical intersection is characterized by a twisted geometry which allows a subsequent photoisomerization. Transient absorption measurements confirmed the formation of a photoisomer in unpolar solvents, while the measurements of fluorescence quantum yields at low temperature demonstrated the existence of an activation energy barrier.…
Author: | Joscha Hoche, Alexander Schulz, Lysanne Monika Dietrich, Alexander Humeniuk, Matthias Stolte, David Schmidt, Tobias Brixner, Frank WürthnerORCiDGND, Roland Mitric |
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URN: | urn:nbn:de:bvb:20-opus-198707 |
Document Type: | Journal article |
Faculties: | Fakultät für Chemie und Pharmazie / Institut für Physikalische und Theoretische Chemie |
Language: | English |
Parent Title (English): | Chemical Science |
Year of Completion: | 2019 |
Volume: | 10 |
Pagenumber: | 11013 |
Source: | Chemical Science, 2019,10, 11013-11022. https://doi.org/10.1039/C9SC05012D |
URL: | https://doi.org/10.1039/C9SC05012D |
Dewey Decimal Classification: | 5 Naturwissenschaften und Mathematik / 54 Chemie / 541 Physikalische Chemie |
Tag: | solvent-dependent fluorescence yield |
Release Date: | 2020/01/28 |
EU-Project number / Contract (GA) number: | 646737 |
OpenAIRE: | OpenAIRE |
Licence (German): | CC BY: Creative-Commons-Lizenz: Namensnennung |