Origin of the Two Bands in the B800 Ring and Their Involvement in the Energy Transfer Network of Allochromatium vinosum

Schröter, Marco; Alcocer, Marcelo J.  P.; Cogdell, Richard J.; Kühn, Oliver; Zigmantas, Donatas

doi:10.1021/acs.jpclett.8b00438

Origin of the Two Bands in the B800 Ring and Their Involvement in the Energy Transfer Network of Allochromatium vinosum

Journal Article · Wed Feb 28 00:00:00 EST 2018 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.8b00438· OSTI ID:1470602

^[1]; Alcocer, Marcelo J. P. ^[2]; Cogdell, Richard J. ^[3]; Kühn, Oliver ^[4]; ^[2]

Univ. of Rostock (Germany). Inst. of Physics; Lund Univ. (Sweden). Dept. of Chemical Physics
Lund Univ. (Sweden). Dept. of Chemical Physics
Univ. of Glasgow, Scotland (United Kingdom). Inst. of Molecular, Cell and Systems Biology, College of Medical, Veterinary and Life Sciences
Univ. of Rostock (Germany). Inst. of Physics

Bacterial photosynthesis features robust and adaptable energy-harvesting processes in which light-harvesting proteins play a crucial role. The peripheral light-harvesting complex of the purple bacterium Allochromatium vinosum is particularly distinct, featuring a double peak structure in its B800 absorption band. Two hypotheses—not necessarily mutually exclusive—concerning the origin of this splitting have been proposed; either two distinct B800 bacteriochlorophyll site energies are involved, or an excitonic dimerization of bacteriochlorophylls within the B800 ring takes place. Through the use of two-dimensional electronic spectroscopy, we present unambiguous evidence that excitonic interaction shapes the split band. We further identify and characterize all of the energy transfer pathways within this complex by using a global kinetic fitting procedure. Our approach demonstrates how the combination of two-dimensional spectral resolution and self-consistent fitting allows for extraction of information on light-harvesting processes, which would otherwise be inaccessible due to signal congestion.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0001035

OSTI ID:: 1470602

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 6 Vol. 9; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems Kunsel, Tenzin; Tiwari, Vivek; Matutes, Yassel Acosta The Journal of Physical Chemistry B, Vol. 123, Issue 2 https://doi.org/10.1021/acs.jpcb.8b10176	journal	December 2018
Before Förster. Initial excitation in photosynthetic light harvesting Karki, Khadga J.; Chen, Junsheng; Sakurai, Atsunori Chemical Science, Vol. 10, Issue 34 https://doi.org/10.1039/c9sc01888c	journal	January 2019
Using fluorescence detected two-dimensional spectroscopy to investigate initial exciton delocalization between coupled chromophores Schröter, Marco; Pullerits, Tõnu; Kühn, Oliver The Journal of Chemical Physics, Vol. 149, Issue 11 https://doi.org/10.1063/1.5046645	journal	September 2018

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