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Single-Molecule Fluorescence Spectroscopy of Photosynthetic Systems

Journal Article · · Chemical Reviews
Photosynthesis begins when a network of pigment–protein complexes captures solar energy and transports it to the reaction center, where charge separation occurs. When necessary (under low light conditions), photosynthetic organisms perform this energy transport and charge separation with near unity quantum efficiency. Remarkably, this high efficiency is maintained under physiological conditions, which include thermal fluctuations of the pigment–protein complexes and changing local environments. These conditions introduce multiple types of heterogeneity in the pigment–protein complexes, including structural heterogeneity, energetic heterogeneity, and functional heterogeneity. Understanding how photosynthetic light-harvesting functions in the face of these fluctuations requires understanding this heterogeneity, which, in turn, requires characterization of individual pigment–protein complexes. Single-molecule spectroscopy has the power to probe individual complexes. In this review, we present an overview of the common techniques for single-molecule fluorescence spectroscopy applied to photosynthetic systems and describe selected experiments on these systems. We discuss how these experiments provide a new understanding of the impact of heterogeneity on light harvesting and thus how these systems are optimized to capture sunlight under physiological conditions.
Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0001088
OSTI ID:
1388262
Journal Information:
Chemical Reviews, Journal Name: Chemical Reviews Journal Issue: 2 Vol. 117; ISSN 0009-2665
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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Dynamics of the Emission Spectrum of a Single LH2 Complex: Interplay of Slow and Fast Nuclear Motions journal April 2006
Laser-Driven Microsecond Temperature Cycles Analyzed by Fluorescence Polarization Microscopy journal April 2006
Comparative Study of Spectral Flexibilities of Bacterial Light-Harvesting Complexes: Structural Implications journal April 2006
How Proteins Trigger Excitation Energy Transfer in the FMO Complex of Green Sulfur Bacteria journal October 2006
Low-Temperature Fluorescence from Single Chlorosomes, Photosynthetic Antenna Complexes of Green Filamentous and Sulfur Bacteria journal November 2006
Single-Molecule Spectroscopic Characterization of Light-Harvesting 2 Complexes Reconstituted into Model Membranes journal July 2007
An Oxygen Scavenging System for Improvement of Dye Stability in Single-Molecule Fluorescence Experiments journal March 2008
Spectral Heterogeneity in Single Light-harvesting Chlorosomes from Green Sulfur Photosynthetic Bacterium Chlorobium tepidum¶ journal April 2002
Presence of Exclusively Bacteriochlorophyll-c Containing Substrain in the Culture of Green Sulfur Photosynthetic Bacterium Chlorobium vibrioforme Strain NCIB 8327 Producing Bacteriochlorophyll-d journal January 2003
Photonic Methods to Enhance Fluorescence Correlation Spectroscopy and Single Molecule Fluorescence Detection journal January 2010
The structure of plant photosystem I super-complex at 2.8 Å resolution journal June 2015

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Robust light harvesting by a noisy antenna journal January 2018
Photoinduced processes in nucleic acids and proteins: concluding remarks journal January 2018
trans -A 2 B-corrole bearing 2,3-di(2-pyridyl)quinoxaline (DPQ)/phenothiazine moieties: synthesis, characterization, electrochemistry and photophysics journal January 2018
Advanced space- and time-resolved techniques for photocatalyst studies journal January 2020
Waveguide-based chemo- and biosensors: complex emulsions for the detection of caffeine and proteins journal January 2019
Microsecond and millisecond dynamics in the photosynthetic protein LHCSR1 observed by single-molecule correlation spectroscopy journal May 2019
The future of quantum biology journal November 2018
Delocalized excitons in natural light-harvesting complexes journal August 2018
Delocalized excitons in natural light harvesting complexes text January 2018