Publikation: Ultrafast electron transfer, recombination and spin dynamics
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The quenching of excited singlet methylene blue (1MB+) by N,N-dimethylaminomethylferrocene (FcN) in acetonitrile at room temperature has been studied using femtosecond pump-probe absorption spectroscopy. At high FcN concentration static quenching via an intermolecular electron transfer mechanism constitutes the predominating decay channel for 1MB+. The time constants of the large amplitude components for the forward electron transfer from FcN donor to 1MB+* and the subsequent recombination process recovering the ground states have been determined to be 390 fs and 1 ps, respectively. Thus, the majority of radical pairs has recombined before paramagnetic relaxation induces spin mixing giving rise to triplet-phased radical pairs. These can escape geminate recombination as the system does not offer low-lying local triplet states to be occupied in the recombination process.
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GILCH, Peter, Florian PÖLLINGER-DAMMER, Ulrich STEINER, Maria Elisabeth MICHEL-BEYERLE, 1997. Ultrafast electron transfer, recombination and spin dynamics. In: Chemical Physics Letters. 1997, 275(3-4), pp. 339-348. ISSN 0009-2614. Available under: doi: 10.1016/S0009-2614(97)00755-0BibTex
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title={Ultrafast electron transfer, recombination and spin dynamics},
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journal={Chemical Physics Letters},
pages={339--348},
author={Gilch, Peter and Pöllinger-Dammer, Florian and Steiner, Ulrich and Michel-Beyerle, Maria Elisabeth}
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<dcterms:abstract xml:lang="eng">The quenching of excited singlet methylene blue (1MB+*) by N,N-dimethylaminomethylferrocene (FcN) in acetonitrile at room temperature has been studied using femtosecond pump-probe absorption spectroscopy. At high FcN concentration static quenching via an intermolecular electron transfer mechanism constitutes the predominating decay channel for 1MB+*. The time constants of the large amplitude components for the forward electron transfer from FcN donor to 1MB+* and the subsequent recombination process recovering the ground states have been determined to be 390 fs and 1 ps, respectively. Thus, the majority of radical pairs has recombined before paramagnetic relaxation induces spin mixing giving rise to triplet-phased radical pairs. These can escape geminate recombination as the system does not offer low-lying local triplet states to be occupied in the recombination process.</dcterms:abstract>
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