Self-Assembled Light-Harvesting System from Chromophores in Lipid Vesicles

Sahin, Tuba; Harris, Michelle A.; Vairaprakash, Pothiappan; Niedzwiedzki, Dariusz M.; Subramanian, Vijaya; Shreve, Andrew P.; Bocian, David F.; Holten, Dewey; Lindsey, Jonathan S.

doi:10.1021/acs.jpcb.5b04841

Title: Self-Assembled Light-Harvesting System from Chromophores in Lipid Vesicles

Journal Article · Fri Jul 31 00:00:00 EDT 2015 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI:https://doi.org/10.1021/acs.jpcb.5b04841· OSTI ID:1386028

Sahin, Tuba ^[1]; Harris, Michelle A. ^[2]; Vairaprakash, Pothiappan ^[1]; Niedzwiedzki, Dariusz M. ^[1]; Subramanian, Vijaya ^[3]; Shreve, Andrew P. ^[3]; Bocian, David F. ^[4]; Holten, Dewey ^[2]; Lindsey, Jonathan S. ^[1]

North Carolina State Univ., Raleigh, NC (United States)
Washington Univ., St. Louis, MO (United States)
Univ. of New Mexico, Albuquerque, NM (United States)
Univ. of California, Riverside, CA (United States)

Lipid vesicles are used as the organizational structure of self-assembled light-harvesting systems. Following analysis of 17 chromophores, six were selected for inclusion in vesicle-based antennas. The complementary absorption features of the chromophores span the near-ultraviolet, visible, and near-infrared region. Although the overall concentration of the pigments is low (~1 μM for quantitative spectroscopic studies) in a cuvette, the lipid-vesicle system affords high concentration (≥10 mM) in the bilayer for efficient energy flow from donor to acceptor. Energy transfer was characterized in 13 representative binary mixtures using static techniques (fluorescence–excitation versus absorptance spectra, quenching of donor fluorescence, modeling emission spectra of a mixture versus components) and time-resolved spectroscopy (fluorescence, ultrafast absorption). Binary donor–acceptor systems that employ a boron-dipyrrin donor (S₀ ↔ S₁ absorption/emission in the blue-green) and a chlorin or bacteriochlorin acceptor (S₀ ↔ S₁ absorption/emission in the red or near-infrared) have an average excitation-energy-transfer efficiency (Φ_EET) of ~50%. Binary systems with a chlorin donor and a chlorin or bacteriochlorin acceptor have Φ_EET ~ 85%. The differences in Φ_EET generally track the donor-fluorescence/acceptor-absorption spectral overlap within a dipole–dipole coupling (Förster) mechanism. Substantial deviation from single-exponential decay of the excited donor (due to the dispersion of donor–acceptor distances) is expected and observed. The time profiles and resulting Φ_EET are modeled on the basis of (Förster) energy transfer between chromophores relatively densely packed in a two-dimensional compartment. Initial studies of two ternary and one quaternary combination of chromophores show the enhanced spectral coverage and energy-transfer efficacy expected on the basis of the binary systems. Collectively, this approach may provide one of the simplest designs for self-assembled light-harvesting systems that afford broad solar collection and efficient energy transfer.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC); Washington Univ., St. Louis, MO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001035

OSTI ID:: 1386028

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Vol. 119, Issue 32; Related Information: PARC partners with Washington University in St. Louis (lead); University of California, Riverside; University of Glasgow, UK; Los Alamos National Laboratory; University of New Mexico; New Mexico Corsortium; North Carolina State University; Northwestern University; Oak Ridge National Laboratory; University of Pennsylvania; Sandia National Laboratories; University of Sheffield, UK; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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Title: Self-Assembled Light-Harvesting System from Chromophores in Lipid Vesicles

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