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Optimal Energy Transfer in Light-Harvesting Systems

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      Abstract

      Photosynthesis is one of the most essential biological processes in which specialized pigment-protein complexes absorb solar photons, and with a remarkably high efficiency, guide the photo-induced excitation energy toward the reaction center to subsequently trigger its conversion to chemical energy. In this work, we review the principles of optimal energy transfer in various natural and artificial light harvesting systems. We begin by presenting the guiding principles for optimizing the energy transfer efficiency in systems connected to dissipative environments, with particular attention paid to the potential role of quantum coherence in light harvesting systems. We will comment briefly on photo-protective mechanisms in natural systems that ensure optimal functionality under varying ambient conditions. For completeness, we will also present an overview of the charge separation and electron transfer pathways in reaction centers. Finally, recent theoretical and experimental progress on excitation energy transfer, charge separation, and charge transport in artificial light harvesting systems is delineated, with organic solar cells taken as prime examples.

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      Polymer Photovoltaic Cells: Enhanced Efficiencies via a Network of Internal Donor-Acceptor Heterojunctions

       G. Yu,  Li Gao,  J Hummelen (1996)
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        Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems.

        Photosynthetic complexes are exquisitely tuned to capture solar light efficiently, and then transmit the excitation energy to reaction centres, where long term energy storage is initiated. The energy transfer mechanism is often described by semiclassical models that invoke 'hopping' of excited-state populations along discrete energy levels. Two-dimensional Fourier transform electronic spectroscopy has mapped these energy levels and their coupling in the Fenna-Matthews-Olson (FMO) bacteriochlorophyll complex, which is found in green sulphur bacteria and acts as an energy 'wire' connecting a large peripheral light-harvesting antenna, the chlorosome, to the reaction centre. The spectroscopic data clearly document the dependence of the dominant energy transport pathways on the spatial properties of the excited-state wavefunctions of the whole bacteriochlorophyll complex. But the intricate dynamics of quantum coherence, which has no classical analogue, was largely neglected in the analyses-even though electronic energy transfer involving oscillatory populations of donors and acceptors was first discussed more than 70 years ago, and electronic quantum beats arising from quantum coherence in photosynthetic complexes have been predicted and indirectly observed. Here we extend previous two-dimensional electronic spectroscopy investigations of the FMO bacteriochlorophyll complex, and obtain direct evidence for remarkably long-lived electronic quantum coherence playing an important part in energy transfer processes within this system. The quantum coherence manifests itself in characteristic, directly observable quantum beating signals among the excitons within the Chlorobium tepidum FMO complex at 77 K. This wavelike characteristic of the energy transfer within the photosynthetic complex can explain its extreme efficiency, in that it allows the complexes to sample vast areas of phase space to find the most efficient path.
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          Conjugated polymer-based organic solar cells.

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            Author and article information

            Affiliations
            Division of Materials Science, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore; E-Mails: CHEN0846@ 123456e.ntu.edu.sg (L.C.); pmshenai@ 123456ntu.edu.sg (P.S.); M130048@ 123456e.ntu.edu.sg (F.Z.); SOMO0001@ 123456e.ntu.edu.sg (A.S.)
            Author notes
            [†]

            These authors contributed equally to this work.

            [* ]Author to whom correspondence should be addressed; E-Mail: YZhao@ 123456ntu.edu.sg ; Tel.: +65-6513-7990; Fax.: +65-6790-9081.
            Contributors
            Role: Academic Editor
            Journal
            Molecules
            Molecules
            molecules
            Molecules
            MDPI
            1420-3049
            20 August 2015
            August 2015
            : 20
            : 8
            : 15224-15272
            26307957
            6332264
            10.3390/molecules200815224
            molecules-20-15224
            (Academic Editor)
            © 2015 by the authors.

            Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution license ( http://creativecommons.org/licenses/by/4.0/).

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