Dichotomous Disorder versus Excitonic Splitting of the B800 Band of Allochromatium vinosum
Abstract
The purple bacterium of Allochromatium vinosum has a distinct double peak structure of the 800 nm band (B800). Several hypotheses were proposed in the literature to explain its origin. Although recent 77 K two-dimensional electronic spectroscopy (2DES) data could neither refute or validate previous findings that the two B800 sub-bands are due to different site-energies (most likely due weakly and strongly hydrogen bonded B800 BChls [A. Kell et al., J. Phys. Chem. B 2017, 121, 9999]), the authors concluded that strong excitonic coupling of dimerized bacteriochlorophylls (BChls) within the B800 ring is largely responsible for the B800 split [M. Schroter et al., J. Phys. Chem. Lett. 2018, 9, 1340]. Here it is demonstrated that the latter is incorrect and excitonic interactions between BChls in the B800 ring, though present, are weak. This conclusion is based on an exciton model with dichotomous protein conformation disorder. We show that complementary data provided by hole burning (HB) spectroscopy, 2DES, and modeling studies provide a more comprehensive picture on the origin of the B800 band split. Energy transfer pathways from B800B → B800R, B800B → B850 and B800R → B850 revealed by HB spectroscopy are compared to those obtained via 2DES.
- Publication Date:
- Research Org.:
- Kansas State Univ., Manhattan, KS (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1539331
- Grant/Contract Number:
- SC0006678
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry Letters
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 14; Journal ID: ISSN 1948-7185
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; absorption; absorption spectroscopy; energy; fluorescence resonance energy transfer; peptides and proteins
Citation Formats
Kell, Adam, Khmelnitskiy, Anton, Jassas, Mahboobe, and Jankowiak, Ryszard. Dichotomous Disorder versus Excitonic Splitting of the B800 Band of Allochromatium vinosum. United States: N. p., 2018.
Web. doi:10.1021/acs.jpclett.8b01584.
Kell, Adam, Khmelnitskiy, Anton, Jassas, Mahboobe, & Jankowiak, Ryszard. Dichotomous Disorder versus Excitonic Splitting of the B800 Band of Allochromatium vinosum. United States. https://doi.org/10.1021/acs.jpclett.8b01584
Kell, Adam, Khmelnitskiy, Anton, Jassas, Mahboobe, and Jankowiak, Ryszard. Mon .
"Dichotomous Disorder versus Excitonic Splitting of the B800 Band of Allochromatium vinosum". United States. https://doi.org/10.1021/acs.jpclett.8b01584. https://www.osti.gov/servlets/purl/1539331.
@article{osti_1539331,
title = {Dichotomous Disorder versus Excitonic Splitting of the B800 Band of Allochromatium vinosum},
author = {Kell, Adam and Khmelnitskiy, Anton and Jassas, Mahboobe and Jankowiak, Ryszard},
abstractNote = {The purple bacterium of Allochromatium vinosum has a distinct double peak structure of the 800 nm band (B800). Several hypotheses were proposed in the literature to explain its origin. Although recent 77 K two-dimensional electronic spectroscopy (2DES) data could neither refute or validate previous findings that the two B800 sub-bands are due to different site-energies (most likely due weakly and strongly hydrogen bonded B800 BChls [A. Kell et al., J. Phys. Chem. B 2017, 121, 9999]), the authors concluded that strong excitonic coupling of dimerized bacteriochlorophylls (BChls) within the B800 ring is largely responsible for the B800 split [M. Schroter et al., J. Phys. Chem. Lett. 2018, 9, 1340]. Here it is demonstrated that the latter is incorrect and excitonic interactions between BChls in the B800 ring, though present, are weak. This conclusion is based on an exciton model with dichotomous protein conformation disorder. We show that complementary data provided by hole burning (HB) spectroscopy, 2DES, and modeling studies provide a more comprehensive picture on the origin of the B800 band split. Energy transfer pathways from B800B → B800R, B800B → B850 and B800R → B850 revealed by HB spectroscopy are compared to those obtained via 2DES.},
doi = {10.1021/acs.jpclett.8b01584},
journal = {Journal of Physical Chemistry Letters},
number = 14,
volume = 9,
place = {United States},
year = {Mon Jun 25 00:00:00 EDT 2018},
month = {Mon Jun 25 00:00:00 EDT 2018}
}
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Works referenced in this record:
On Light-Induced Photoconversion of B800 Bacteriochlorophylls in the LH2 Antenna of the Purple Sulfur Bacterium Allochromatium vinosum
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Works referencing / citing this record:
Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems
journal, December 2018
- Kunsel, Tenzin; Tiwari, Vivek; Matutes, Yassel Acosta
- The Journal of Physical Chemistry B, Vol. 123, Issue 2