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  Quantum coherence controls the charge separation in a prototypical artificial light-harvesting system

Rozzi, C. A., Falke, S. M., Spallanzani, N., Rubio, A., Molinari, E., Brida, D., et al. (2013). Quantum coherence controls the charge separation in a prototypical artificial light-harvesting system. Nature Communications, 4: 1602. doi:doi:10.1038/ncomms2603.

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 Creators:
Rozzi, Carlo Andrea1, Author
Falke, Sarah Maria2, Author
Spallanzani, Nicola1, 3, Author
Rubio, Angel4, 5, Author           
Molinari, Elisa1, 3, Author
Brida, Daniele6, Author
Maiuri, Margherita6, Author
Cerullo, Giulio6, Author
Schramm, Heiko7, Author
Christoffers, Jens7, Author
Lienau, Christoph2, Author
Affiliations:
1Istituto Nanoscienze – CNR, Centro S3, via Campi 213a, 41125 Modena, Italy, ou_persistent22              
2Institut für Physik and Center of Interface Science, Carl von Ossietzky Universität, 26111 Oldenburg, Germany, ou_persistent22              
3Dipartimento di Fisica, Università di Modena e Reggio Emilia, via Campi 213a, 41125 Modena, Italy, ou_persistent22              
4Theory, Fritz Haber Institute, Max Planck Society, Berlin, DE, ou_634547              
5Nano-Bio Spectroscopy Group and ETSF Scientific Development Centre, Departamento de F, ou_persistent22              
6IFN-CNR, Dipartimento di Fisica, Politecnico di Milano, 20133 Milano, Italy, ou_persistent22              
7Institut für Chemie and Center of Interface Science, Carl von Ossietzky Universität, 26111 Oldenburg, Germany, ou_persistent22              

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 Abstract: The efficient conversion of light into electricity or chemical fuels is a fundamental challenge. In artificial photosynthetic and photovoltaic devices, this conversion is generally thought to happen on ultrafast, femto-to-picosecond timescales and to involve an incoherent electron transfer process. In some biological systems, however, there is growing evidence that the coherent motion of electronic wavepackets is an essential primary step, raising questions about the role of quantum coherence in artificial devices. Here we investigate the primary charge-transfer process in a supramolecular triad, a prototypical artificial reaction centre. Combining high time-resolution femtosecond spectroscopy and time-dependent density functional theory, we provide compelling evidence that the driving mechanism of the photoinduced current generation cycle is a correlated wavelike motion of electrons and nuclei on a timescale of few tens of femtoseconds. We highlight the fundamental role of the interface between chromophore and charge acceptor in triggering the coherent wavelike electron-hole splitting.

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Language(s): eng - English
 Dates: 2012-06-062013-02-142013-03-19
 Publication Status: Published online
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: doi:10.1038/ncomms2603
 Degree: -

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Project name : DYNAMO - Dynamical processes in open quantum systems: pushing the frontiers of theoretical spectroscopy
Grant ID : 267374
Funding program : Funding Programme 7 (FP7)
Funding organization : European Commission (EC)

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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: 4 Sequence Number: 1602 Start / End Page: - Identifier: ISSN: 2041-1723
CoNE: https://pure.mpg.de/cone/journals/resource/2041-1723