Journal
NATURE COMMUNICATIONS
Volume 4, Issue -, Pages -Publisher
NATURE RESEARCH
DOI: 10.1038/ncomms2603
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Funding
- European Community through the CRONOS project [280879]
- CINECA, Italy, ISCRA project [HP10BWZPJA]
- Deutsche Forschungsgemeinschaft [SPP1391]
- Deutsche Forschungsgemeinschaft (DFG-NSF Materials World Network)
- Korea Foundation for International Cooperation of Science and Technology (Global Research Laboratory Project) [K20815000003]
- Stiftung der Metallindustrie im Nord-Westen
- European Research Council Advanced Grant DYNamo [267374]
- Spanish MICINN [FIS2010-65702-C02-01, PIB2010US-00652, /CSD2010-00044/]
- ACI-Promociona [ACI2009-1036]
- Grupos Consolidados UPV/EHU del Gobierno Vasco [IT-319-07]
- PRIN programme [2008JKBBK4]
- European Research Council Advanced Grant STRATUS [291198]
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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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