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Ultrafast Intramolecular Relaxation and Wave-Packet Motion in a Ruthenium-Based Supramolecular Photocatalyst
Abstract
The hydrogen-evolving photocatalyst [(tbbpy)2 Ru(tpphz)Pd(Cl)2 ](2+) (tbbpy=4,4'-di-tert-butyl-2,2'-bipyridine, tpphz=tetrapyrido[3,2-a:2',3'-c:3'',2''-h:2''',3'''-j]phenazine) shows excitation-wavelength-dependent catalytic activity, which has been correlated to the localization of the initial excitation within the coordination sphere. In this contribution the excitation-wavelength dependence of the early excited-state relaxation and the occurrence of vibrational coherences are investigated by sub-20 fs transient absorption spectroscopy and DFT/TDDFT calculations. The comparison with the mononuclear precursor [(tbbpy)2 Ru(tpphz)](2+) highlights the influence of the catalytic center on these ultrafast processes. Only in the presence of the second metal center, does the excitation of a (1) MLCT state localized on the central part of the tpphz bridge lead to coherent wave-packet motion in the excited state.
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Authors (9)
-
Maria WäCHTLER
- Jena IPHT
-
Stephan Kupfer
- University Jena Institute of Physical Chemistry and Abbe Center of Photonics
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Margherita Maiuri
- IFN-CNR Dipartimento di Fisica
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Daniele Brida
- University of Konstanz Department of Physics and Center for Applied Photonics
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Jürgen Popp
- Jena IPHT
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Sven Rau
- Universitety of Ulm Institute of Inorganic Chemistry
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Giulio Cerullo
- IFN-CNR Dipartimento di Fisica
-
Benjamin Dietzek
- Jena IPHT
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Details
- Category:
- Articles
- Type:
- artykuł w czasopiśmie wyróżnionym w JCR
- Published in:
-
CHEMISTRY-A EUROPEAN JOURNAL
no. 21,
edition 21,
pages 7668 - 7674,
ISSN: 0947-6539 - Language:
- English
- Publication year:
- 2015
- Bibliographic description:
- Wächtler M., Guthmuller J., Kupfer S., Maiuri M., Brida D., Popp J., Rau S., Cerullo G., Dietzek B.: Ultrafast Intramolecular Relaxation and Wave-Packet Motion in a Ruthenium-Based Supramolecular Photocatalyst// CHEMISTRY-A EUROPEAN JOURNAL. -Vol. 21, iss. 21 (2015), s.7668-7674
- DOI:
- Digital Object Identifier (open in new tab) 10.1002/chem.201406350
- Verified by:
- Gdańsk University of Technology
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