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doi:10.22028/D291-35449
Titel: | Solvent‐Controlled Intermolecular Proton‐Transfer Follows an Irreversible Eigen‐Weller Model from fs to ns |
VerfasserIn: | Grandjean, Alexander Pérez Lustres, J. Luis Jung, Gregor |
Sprache: | Englisch |
Titel: | ChemPhotoChem |
Bandnummer: | 5 |
Heft: | 12 |
Seiten: | 1094– 1105 |
Verlag/Plattform: | Wiley |
Erscheinungsjahr: | 2021 |
Freie Schlagwörter: | Eigen-Weller model excited states proton transfer solvent relaxation transient absorption spectroscopy |
DDC-Sachgruppe: | 500 Naturwissenschaften |
Dokumenttyp: | Journalartikel / Zeitschriftenartikel |
Abstract: | Intermolecular Proton Transfer (PT) dynamics can be best studied by optical spectroscopy, which can cover the vast timescale spanned by the process. PT in a hydrogen bonding complex between a pyranine-based photoacid and a trialkyl-phosphine oxide is addressed. The photoreaction is traced with the help of femtosecond transient absorption and picosecond-resolved fluorescence. Characteristic kinetics and spectra of the intervening species are isolated by global analysis and spectral decomposition of time-resolved fluorescence. It is found that the shared proton shifts towards the phosphine site upon photoexcitation in acetonitrile. The process occurs on the sub-picosecond timescale, essentially, under solvent control. Despite the ultrafast rate, an equilibrium between the complex and the hydrogen-bonded ion pair (HBIP) is established. Further reaction steps are delayed to the nanosecond timescale, where formation of the excited deprotonated form is observed. The far-reaching consistency between the various methods supports an irreversible Eigen-Weller mechanism in the excited state. |
DOI der Erstveröffentlichung: | 10.1002/cptc.202100177 |
Link zu diesem Datensatz: | urn:nbn:de:bsz:291--ds-354493 hdl:20.500.11880/32372 http://dx.doi.org/10.22028/D291-35449 |
ISSN: | 2367-0932 |
Datum des Eintrags: | 9-Feb-2022 |
Bezeichnung des in Beziehung stehenden Objekts: | Supporting Information |
In Beziehung stehendes Objekt: | https://chemistry-europe.onlinelibrary.wiley.com/action/downloadSupplement?doi=10.1002%2Fcptc.202100177&file=cptc202100177-sup-0001-misc_information.pdf |
Fakultät: | NT - Naturwissenschaftlich- Technische Fakultät |
Fachrichtung: | NT - Chemie |
Professur: | NT - Prof. Dr. Gregor Jung |
Sammlung: | SciDok - Der Wissenschaftsserver der Universität des Saarlandes |
Dateien zu diesem Datensatz:
Datei | Beschreibung | Größe | Format | |
---|---|---|---|---|
ChemPhotoChem - 2021 - Grandjean - Solvent‐Controlled Intermolecular Proton‐Transfer Follows an Irreversible Eigen‐Weller.pdf | 4,97 MB | Adobe PDF | Öffnen/Anzeigen |
Diese Ressource wurde unter folgender Copyright-Bestimmung veröffentlicht: Lizenz von Creative Commons