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

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2015
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Wächtler, Maria
Guthmuller, Julien
Kupfer, Stephan
Maiuri, Margherita
Popp, Jürgen
Rau, Sven
Cerullo, Giulio
Dietzek, Benjamin
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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.

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530 Physik
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coherent vibrational motion, DFT, photophysics, ruthenium, time-resolved spectroscopy
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ISO 690WÄCHTLER, 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. 2015, 21(21), pp. 7668-7674. ISSN 0947-6539. eISSN 1521-3765. Available under: doi: 10.1002/chem.201406350
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@article{Wachtler2015-03-20Ultra-30813,
  year={2015},
  doi={10.1002/chem.201406350},
  title={Ultrafast Intramolecular Relaxation and Wave‐Packet Motion in a Ruthenium‐Based Supramolecular Photocatalyst},
  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}
}
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