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Ultrafast Intramolecular Relaxation and Wave‐Packet Motion in a Ruthenium‐Based Supramolecular Photocatalyst

Ultrafast Intramolecular Relaxation and Wave‐Packet Motion in a Ruthenium‐Based Supramolecular Photocatalyst

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WÄCHTLER, Maria, Julien GUTHMULLER, Stephan KUPFER, Margherita MAIURI, Daniele BRIDA, Jürgen POPP, Sven RAU, Giulio CERULLO, Benjamin DIETZEK, 2015. Ultrafast Intramolecular Relaxation and Wave‐Packet Motion in a Ruthenium‐Based Supramolecular Photocatalyst. In: Chemistry - A European Journal. 21(21), pp. 7668-7674. ISSN 0947-6539. eISSN 1521-3765. Available under: doi: 10.1002/chem.201406350

@article{Wachtler2015-03-20Ultra-30813, title={Ultrafast Intramolecular Relaxation and Wave‐Packet Motion in a Ruthenium‐Based Supramolecular Photocatalyst}, year={2015}, doi={10.1002/chem.201406350}, number={21}, volume={21}, issn={0947-6539}, journal={Chemistry - A European Journal}, pages={7668--7674}, author={Wächtler, Maria and Guthmuller, Julien and Kupfer, Stephan and Maiuri, Margherita and Brida, Daniele and Popp, Jürgen and Rau, Sven and Cerullo, Giulio and Dietzek, Benjamin} }

2015-03-20 Maiuri, Margherita Kupfer, Stephan The hydrogen-evolving photocatalyst [(tbbpy)<sub>2</sub>Ru(tpphz)Pd(Cl)<sub>2</sub>]<sup>2+</sup> (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)<sub>2</sub>Ru(tpphz)]<sup>2</sup>+ 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 <sup>1</sup>MLCT state localized on the central part of the tpphz bridge lead to coherent wave-packet motion in the excited state. Dietzek, Benjamin 2015-04-23T09:49:09Z Popp, Jürgen Guthmuller, Julien Cerullo, Giulio Maiuri, Margherita Brida, Daniele Ultrafast Intramolecular Relaxation and Wave‐Packet Motion in a Ruthenium‐Based Supramolecular Photocatalyst eng Popp, Jürgen Brida, Daniele Wächtler, Maria Guthmuller, Julien Cerullo, Giulio Wächtler, Maria Dietzek, Benjamin 2015-04-23T09:49:09Z Rau, Sven Rau, Sven Kupfer, Stephan

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