Enhanced light-harvesting capacity by micellar assembly of free accessory chromophores and LH1-like antennas

Michelle A. Harris, Tuba Sahin, Jianbing Jiang, Pothiappan Vairaprakash, Pamela S Parkes-Loach, Dariusz M. Niedzwiedzki, Christine Kirmaier, Paul A Loach, David F. Bocian*, Dewey Holten, Jonathan S. Lindsey

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

11 Scopus citations

Abstract

Biohybrid light-harvesting antennas are an emerging platform technology with versatile tailorability for solar-energy conversion. These systems combine the proven peptide scaffold unit utilized for light harvesting by purple photosynthetic bacteria with attached synthetic chromophores to extend solar coverage beyond that of the natural systems. Herein, synthetic unattached chromophores are employed that partition into the organized milieu (e.g. detergent micelles) that house the LH1- like biohybrid architectures. The synthetic chromophores include a hydrophobic boron-dipyrrin dye (A1) and an amphiphilic bacteriochlorin (A2), which transfer energy with reasonable efficiency to the bacteriochlorophyll acceptor array (B875) of the LH1-like cyclic oligomers. The energy-transfer efficiencies are markedly increased upon covalent attachment of a bacteriochlorin (B1 or B2) to the peptide scaffold, where the latter likely acts as an energy-transfer relay site for the (potentially diffusing) free chromophores. The efficiencies are consistent with a F€orster (through-space) mechanism for energy transfer. The overall energy-transfer efficiency from the free chromophores via the relay to the target site can approach those obtained previously by relay-assisted energy transfer from chromophores attached at distant sites on the peptides. Thus, the use of free accessory chromophores affords a simple design to enhance the overall light-harvesting capacity of biohybrid LH1-like architectures.

Original languageEnglish (US)
Pages (from-to)1264-1276
Number of pages13
JournalPhotochemistry and Photobiology
Volume90
Issue number6
DOIs
StatePublished - Jan 1 2014

ASJC Scopus subject areas

  • Biochemistry
  • Physical and Theoretical Chemistry

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