Berlin 2012 – wissenschaftliches Programm
HL 68.1: Vortrag
Mittwoch, 28. März 2012, 17:45–18:00, ER 270
Quantum coherence controls the charge separation in a prototypical artificial light harvesting system — •Sarah Maria Falke1, Carlo Andrea Rozzi2, Nicola Spallanzani2, Angel Rubio3, Elisa Molinari2, Daniele Brida4, Margherita Maiuri4, Giulio Cerullo4, Heiko Schramm1, Jens Christoffers1, and Christoph Lienau1 — 1Carl von Ossietzky Universität, Oldenburg, Germany — 2CNR, Centro S3, Modena, Italy — 3Fritz-Haber-Institut, Berlin, Germany — 4IFN-CNR, Politecnico di Milano, Italy
In artificial light harvesting systems the conversion of light into electrical or chemical energy happens on the femtosecond time scale and is thought to involve the incoherent jump of an electron from the optical absorber to an electron acceptor. Here we investigate the primary process of electronic charge transfer dynamics in a supramolecular triad, a prototypical elementary component for an artificial photosynthetic/photovoltaic system. Combining coherent femtosecond spectroscopy and first-principles quantum dynamics simulations, we provide compelling evidence that the driving mechanism of the photoinduced current generation cycle is a quantum correlated wavelike motion of electrons and nuclei on a timescale of few tens of femtoseconds. Our work highlights the fundamental role played by the chemical interface between the light-absorbing chromophore and the charge acceptor in triggering the coherent wavelike electron-hole splitting.