Quantum coherence controls the charge separation in a prototypical artificial light-harvesting system
Open accessAbstract
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. In artificial photosynthetic devices, conversion of light into electricity is thought to involve an incoherent electron transfer process. Rozzi et al.provide evidence for quantum-correlated wavelike motion inducing the ultrafast photoinduced electronic charge transfer in a light-harvesting supramolecular triad.
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Investigations of primary charge transfer in a prototypical artificial reaction centre have revealed correlated wave-like motion of electrons and nuclei on a time scale of a few tens of femtoseconds as a driving mechanism of the photoinduced current generation cycle.
“Investigations of primary charge transfer in a prototypical artificial reaction centre have revealed correlated wave-like motion of electrons and nuclei on a time scale of a few tens of femtoseconds as a driving mechanism of the photoinduced current generation cycle [76].”
From The future of quantum biology (2018) · cites this paper as [76]
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- Authors
- Andrea Rozzi, C., Maria Falke, S., Spallanzani, N., Rubio, A., Molinari, E., Brida, D., Maiuri, M., Cerullo, G., Schramm, H., Christoffers, J., & Lienau, C.
- Affiliations
- University of Modena and Reggio Emilia (IT)
- Politecnico di Milano (IT)
- Carl von Ossietzky Universität Oldenburg (DE)
- Corresponding author
- Lienau, Christoph
- ORCID
- Venue
- Nature Communications
- Published
- 2013-03-19
- Volume
- 4
- Issue
- 1
- Pages
- 1602-1602
- ISSN
- 2041-1723 (ISSN-L)
- PMC
- PMC3615481
- OpenAlex
- W2013765201
- Cited by
- 282
- References
- 52
- Citations by year
- 2026: 7 · 2025: 9 · 2024: 18 · 2023: 15 · 2022: 19 · 2021: 27 · 2020: 22 · 2019: 21 · 2018: 24 · 2017: 26 · 2016: 29 · 2015: 30 · 2014: 23 · 2013: 10 · 2012: 1
- FWCI
- 19.35
- Type
- journal article
- Language
- en
- Open access
- hybrid
- doi.org
- Licence
- Locations
- Nature Communications (publishedVersion, cc-by-nc-nd)
- Europe PMC (PubMed Central) (publishedVersion, cc-by-nc-nd)
- PubMed Central (publishedVersion, cc-by-nc-nd)
- PubMed (publishedVersion)
- IRIS UNIMORE (University of Modena and Reggio Emilia) (submittedVersion, cc-by-nc-nd)
- MPG.PuRe (Max Planck Society) (submittedVersion, cc-by-nc-nd)
- DIGITAL.CSIC (Spanish National Research Council (CSIC)) (submittedVersion, cc-by-nc-nd)
- IRIS UNIMORE (University of Modena and Reggio Emilia) (submittedVersion, cc-by)
- Virtual Community of Pathological Anatomy (University of Castilla La Mancha) (submittedVersion)
- Funders
- National Science Foundation
- European Commission (280879)
- Deutsche Forschungsgemeinschaft (SPP-1391)
- Eusko Jaurlaritza
- Euskal Herriko Unibertsitatea
- Ministerio de Ciencia e Innovación (CSD2010-00044, PIB2010US-00652)
- FP7 Ideas: European Research Council (267374, 291198)
- Topics
- Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Organic Electronics and Photovoltaics
- Keywords
- quantum coherence, charge separation, artificial light-harvesting systems, photoinduced charge transfer, ultrafast electron dynamics, artificial photosynthesis, femtosecond spectroscopy
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