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Issue 10, 2013
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Integration of multiple chromophores with native photosynthetic antennas to enhance solar energy capture and delivery

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Abstract

Native length bacterial light-harvesting peptides carrying covalently attached designer chromophores have been created that self-assemble with native bacteriochlorophyll a (BChl a) to afford stable antennas with enhanced spectral coverage. Native (or native-like) α- and β-peptides interact with each other and BChl a to form a heterodimeric (αβ-dyad) unit that can then oligomerize to form biohybrid analogs of the bacterial core light-harvesting complex (LH1). Pairs of distinct synthetic chromophores were incorporated in αβ-dyads at selected distances from the BChl a target site (position 0). Two designs were explored. One design used green-yellow absorbing/emitting Oregon Green at the −34 position (toward the N-terminus relative to the BChl a coordination site) of β and orange-red absorbing/emitting Rhodamine Red at the −20 position of α, which combine with BChl a to give homogeneous oligomers. A second design used two different β-peptide conjugates, one with Oregon Green at the −34 position and the second with a near-infrared absorbing/emitting synthetic bacteriochlorin at the −14 position, which combine with α and BChl a to give a heterogeneous mixture of oligomers. The designs afford antennas with ∼45 to ∼60 pigments, provide enhanced spectral coverage across the visible and near-infrared regions relative to native antennas, and accommodate pigments at remote sites that contribute to solar light harvesting via an energy-transfer cascade. The efficiencies of energy-transfer to the BChl a target in the biohybrid antennas are comparable to native antennas, as revealed by static and time-resolved absorption and emission studies. The results show that the biohybrid approach, where designer chromophores are integrated via semisynthesis with native-like scaffolding, constitutes a versatile platform technology for rapid prototyping of antennas for solar energy capture without the laborious synthesis typically required for creating artificial photosynthetic light-harvesting architectures.

Graphical abstract: Integration of multiple chromophores with native photosynthetic antennas to enhance solar energy capture and delivery

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Publication details

The article was received on 30 May 2013, accepted on 29 Jul 2013 and first published on 06 Aug 2013


Article type: Edge Article
DOI: 10.1039/C3SC51518D
Citation: Chem. Sci., 2013,4, 3924-3933
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    Integration of multiple chromophores with native photosynthetic antennas to enhance solar energy capture and delivery

    M. A. Harris, P. S. Parkes-Loach, J. W. Springer, J. Jiang, E. C. Martin, P. Qian, J. Jiao, D. M. Niedzwiedzki, C. Kirmaier, J. D. Olsen, D. F. Bocian, D. Holten, C. N. Hunter, J. S. Lindsey and P. A. Loach, Chem. Sci., 2013, 4, 3924
    DOI: 10.1039/C3SC51518D

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