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Ultrafast transient absorption and solvation of a super-photoacid in acetoneous environments
Knorr, Johannes
, Sülzner, Niklas, Geissler, Bastian, Spies, Christian, Grandjean, Alexander
, Kutta, Roger Jan, Jung, Gregor und Nuernberger, Patrick
(2022)
Ultrafast transient absorption and solvation of a super-photoacid in acetoneous environments.
Photochemical & Photobiological Sciences 21, S. 2179-2192.
Veröffentlichungsdatum dieses Volltextes: 05 Okt 2022 04:50
Artikel
DOI zum Zitieren dieses Dokuments: 10.5283/epub.52995
Zusammenfassung
The phenomenon of photoacidity, i.e., an increase in acidity by several orders of magnitude upon electronic excitation, is frequently encountered in aromatic alcohols capable of transferring a proton to a suitable acceptor. A promising new class of neutral super-photoacids based on pyranine derivatives has been shown to exhibit pronounced solvatochromic effects. To disclose the underlying ...
The phenomenon of photoacidity, i.e., an increase in acidity by several orders of magnitude upon electronic excitation, is frequently encountered in aromatic alcohols capable of transferring a proton to a suitable acceptor. A promising new class of neutral super-photoacids based on pyranine derivatives has been shown to exhibit pronounced solvatochromic effects. To disclose the underlying mechanisms contributing to excited-state proton transfer (ESPT) and the temporal characteristics of solvation and ESPT, we scrutinize the associated ultrafast dynamics of the strongest photoacid of this class, namely tris(1,1,1,3,3,3-hexafluoropropan-2-yl)8-hydroxypyrene-1,3,6-trisulfonate, in acetoneous environment, thereby finding experimental evidence for ESPT even under these adverse conditions for proton transfer. Juxtaposing results from time-correlated single-photon counting and femtosecond transient absorption measurements combined with a complete decomposition of all signal components, i.e., absorption of ground and excited states as well as stimulated emission, we disclose dynamics of solvation, rotational diffusion, and radiative relaxation processes in acetone and identify the relevant steps of ESPT along with the associated time scales.
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| Dokumentenart | Artikel | ||||
| Titel eines Journals oder einer Zeitschrift | Photochemical & Photobiological Sciences | ||||
| Verlag: | Springer | ||||
|---|---|---|---|---|---|
| Ort der Veröffentlichung: | LONDON | ||||
| Band: | 21 | ||||
| Seitenbereich: | S. 2179-2192 | ||||
| Datum | 30 September 2022 | ||||
| Institutionen | Chemie und Pharmazie > Institut für Physikalische und Theoretische Chemie > Lehrstuhl für Physikalische Chemie I > Prof. Dr. Patrick Nürnberger | ||||
| Identifikationsnummer |
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| Stichwörter / Keywords | STATE PROTON-TRANSFER; PHOTOSYNTHETIC REACTION-CENTER; EXCITED-STATE; GEMINATE RECOMBINATION; INTERMOLECULAR PROTON; ENERGY-TRANSFER; POLARIZATION ANISOTROPY; PYRANINE; SOLVENT; DYNAMICS | ||||
| Dewey-Dezimal-Klassifikation | 500 Naturwissenschaften und Mathematik > 540 Chemie | ||||
| Status | Veröffentlicht | ||||
| Begutachtet | Ja, diese Version wurde begutachtet | ||||
| An der Universität Regensburg entstanden | Zum Teil | ||||
| URN der UB Regensburg | urn:nbn:de:bvb:355-epub-529957 | ||||
| Dokumenten-ID | 52995 |
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