Quenching Capabilities of Long-Chain Carotenoids in Light-Harvesting-2 Complexes from Rhodobacter sphaeroides with an Engineered Carotenoid Synthesis Pathway

Dilbeck, Preston L.; Tang, Qun; Mothersole, David J.; Martin, Elizabeth C.; Hunter, C. Neil; Bocian, David F.; Holten, Dewey; Niedzwiedzki, Dariusz M.

doi:10.1021/acs.jpcb.6b03305

Title: Quenching Capabilities of Long-Chain Carotenoids in Light-Harvesting-2 Complexes from Rhodobacter sphaeroides with an Engineered Carotenoid Synthesis Pathway

Journal Article · Fri Jun 10 00:00:00 EDT 2016 · Journal of Physical Chemistry. B

DOI:https://doi.org/10.1021/acs.jpcb.6b03305· OSTI ID:1256529

Dilbeck, Preston L.; Tang, Qun ^[1]; Mothersole, David J. ^[2]; Martin, Elizabeth C. ^[2]; Hunter, C. Neil ^[2]; Bocian, David F. ^[1]; Holten, Dewey; Niedzwiedzki, Dariusz M.

Department of Chemistry, University of California Riverside, Riverside, California 92521, United States
Department of Molecular Biology and Biotechnology, University of Sheffield, Sheffield S10 2TN, United Kingdom

Here, six light-harvesting-2 complexes (LH2) from genetically modified strains of the purple photosynthetic bacterium Rhodobacter (Rb.) sphaeroides were studied using static and ultrafast optical methods and resonance Raman spectroscopy. These strains were engineered to incorporate carotenoids for which the number of conjugated groups (N = N_C=C + N_C=O) varies from 9 to 15. The Rb. sphaeroides strains incorporate their native carotenoids spheroidene (N = 10) and spheroidenone (N = 11), as well as longer-chain analogues including spirilloxanthin (N = 13) and diketospirilloxantion (N = 15) normally found in Rhodospirillum rubrum. Measurements of the properties of the carotenoid first singlet excited state (S1) in antennas from the Rb. sphaeroides set show that carotenoid-bacteriochlorophyll a (BChl a) interactions are similar to those in LH2 complexes from various other bacterial species and thus are not significantly impacted by differences in polypeptide composition. Instead, variations in carotenoid-to-BChl a energy transfer are primarily regulated by the N-determined energy of the carotenoid S₁ excited state, which for long-chain (N ≥ 13) carotenoids is not involved in energy transfer. Furthermore, the role of the long-chain carotenoids switches from a lightharvesting supporter (via energy transfer to BChl a) to a quencher of the BChl a S₁ excited state B850*. This quenching is manifested as a substantial (~2-fold) reduction of the B850* lifetime and the B850* fluorescence quantum yield for LH2 housing the longest carotenoids

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

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

Grant/Contract Number:: SC 0001035; SC0001035

OSTI ID:: 1256529

Alternate ID(s):: OSTI ID: 1258744

Journal Information:: Journal of Physical Chemistry. B, Journal Name: Journal of Physical Chemistry. B Vol. 120 Journal Issue: 24; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 19 works

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Title: Quenching Capabilities of Long-Chain Carotenoids in Light-Harvesting-2 Complexes from Rhodobacter sphaeroides with an Engineered Carotenoid Synthesis Pathway

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