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Observation of robust energy transfer in the photosynthetic protein allophycocyanin using single-molecule pump–probe spectroscopy
Name
Observation_of_robust_energy_transfer_in_the_photo.pdf
Description
Submitted version
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2.45 MB
Format
Adobe PDF
Checksum (MD5)
43867f10a552762fb6dd46b97c8ae2a2
Author(s)
Moya, Raymundo
Norris, Audrey C
Kondo, Toru
Schlau-Cohen, Gabriela S
Date Issued
February 2022
Journal
Nature Chemistry
Publisher
Springer Science and Business Media LLC
Citation
Moya, Raymundo, Norris, Audrey C, Kondo, Toru and Schlau-Cohen, Gabriela S. 2022. "Observation of robust energy transfer in the photosynthetic protein allophycocyanin using single-molecule pump–probe spectroscopy." Nature Chemistry, 14 (2).
Version
Original manuscript
Abstract
Photosynthetic organisms convert sunlight to electricity with near unity quantum efficiency. Absorbed photoenergy transfers through a network of chromophores positioned within protein scaffolds, which fluctuate due to thermal motion. The resultant variation in the individual energy transfer steps has not yet been measured, and so how the efficiency is robust to this variation has not been determined. Here, we describe single-molecule pump-probe spectroscopy with facile spectral tuning and its application to the ultrafast dynamics of single allophycocyanin, a light-harvesting protein from cyanobacteria. We disentangled the energy transfer and energetic relaxation from nuclear motion using the spectral dependence of the dynamics. We observed an asymmetric distribution of timescales for energy transfer and a slower and more heterogeneous distribution of timescales for energetic relaxation, which was due to the impact of the protein environment. Collectively, these results suggest that energy transfer is robust to protein fluctuations, a prerequisite for efficient light harvesting.
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Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
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DOI of Published Version
10.1038/s41557-021-00841-9
