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Science. 2014 May 30;344(6187):1001-5. doi: 10.1126/science.1249771.

Coherent ultrafast charge transfer in an organic photovoltaic blend.

Science (New York, N.Y.)

Sarah Maria Falke, Carlo Andrea Rozzi, Daniele Brida, Margherita Maiuri, Michele Amato, Ephraim Sommer, Antonietta De Sio, Angel Rubio, Giulio Cerullo, Elisa Molinari, Christoph Lienau

Affiliations

  1. Institut für Physik, Carl von Ossietzky Universität, 26129 Oldenburg, Germany. Center of Interface Science, Carl von Ossietzky Universität, 26129 Oldenburg, Germany.
  2. Istituto Nanoscienze-Consiglio Nazionale delle Ricerche (CNR), Centro S3, via Campi 213a, 41125 Modena, Italy.
  3. Istituto di Fotonica e Nanotecnologie-CNR, Dipartimento di Fisica, Politecnico di Milano, 20133 Milano, Italy. Department of Physics and Center for Applied Photonics, University of Konstanz, 78457 Konstanz, Germany.
  4. Istituto di Fotonica e Nanotecnologie-CNR, Dipartimento di Fisica, Politecnico di Milano, 20133 Milano, Italy.
  5. Institut d'Électronique Fondamentale, UMR8622, CNRS, Universitè Paris-Sud, 91405 Orsay, France.
  6. Nano-Bio Spectroscopy Group and European Theoretical Spectroscopy Facility Scientific Development Centre, Departamento Física de Materiales, Universidad del País Vasco (UPV), Centro de Física de Materiales Consejo Superior de Investigaciones Científicas-UPV/Euskal Herriko Unibertsitatea-Materials Physics Center and Donostia International Physics Center, Avenida Tolosa 72, 20018 San Sebastián, Spain. Fritz-Haber-Institut der Max-Planck-Gesellschaft, 14195 Berlin, Germany.
  7. Istituto Nanoscienze-Consiglio Nazionale delle Ricerche (CNR), Centro S3, via Campi 213a, 41125 Modena, Italy. Dipartimento di Scienze Fisiche, Informatiche e Matematiche, Università di Modena e Reggio Emilia, via Campi 213a, 41125 Modena, Italy. [email protected] [email protected].
  8. Institut für Physik, Carl von Ossietzky Universität, 26129 Oldenburg, Germany. Center of Interface Science, Carl von Ossietzky Universität, 26129 Oldenburg, Germany. [email protected] [email protected].

PMID: 24876491 DOI: 10.1126/science.1249771

Abstract

Blends of conjugated polymers and fullerene derivatives are prototype systems for organic photovoltaic devices. The primary charge-generation mechanism involves a light-induced ultrafast electron transfer from the light-absorbing and electron-donating polymer to the fullerene electron acceptor. Here, we elucidate the initial quantum dynamics of this process. Experimentally, we observed coherent vibrational motion of the fullerene moiety after impulsive optical excitation of the polymer donor. Comparison with first-principle theoretical simulations evidences coherent electron transfer between donor and acceptor and oscillations of the transferred charge with a 25-femtosecond period matching that of the observed vibrational modes. Our results show that coherent vibronic coupling between electronic and nuclear degrees of freedom is of key importance in triggering charge delocalization and transfer in a noncovalently bound reference system.

Copyright © 2014, American Association for the Advancement of Science.

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