Brida, Daniele

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

2015-03-20, Wächtler, Maria, Guthmuller, Julien, Kupfer, Stephan, Maiuri, Margherita, Brida, Daniele, Popp, Jürgen, Rau, Sven, Cerullo, Giulio, Dietzek, Benjamin

The hydrogen-evolving photocatalyst [(tbbpy)2Ru(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)2Ru(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 1MLCT state localized on the central part of the tpphz bridge lead to coherent wave-packet motion in the excited state.