Ultra-broadband 2D electronic spectroscopy of carotenoid-bacteriochlorophyll interactions in the LH1 complex of a purple bacterium
Abstract
We investigate the excitation energy transfer (EET) pathways in the photosynthetic light harvesting 1 (LH1) complex of purple bacterium Rhodospirillum rubrum with ultra-broadband two-dimensional electronic spectroscopy (2DES). We employ a 2DES apparatus in the partially collinear geometry, using a passive birefringent interferometer to generate the phase-locked pump pulse pair. This scheme easily lends itself to two-color operation, by coupling a sub-10 fs visible pulse with a sub-15-fs near-infrared pulse. This unique pulse combination allows us to simultaneously track with extremely high temporal resolution both the dynamics of the photoexcited carotenoid spirilloxanthin (Spx) in the visible range and the EET between the Spx and the B890 bacterio-chlorophyll (BChl), whose Qx and Qy transitions peak at 585 and 881 nm, respectively, in the near-infrared. Global analysis of the one-color and two-color 2DES maps unravels different relaxation mechanisms in the LH1 complex: (i) the initial events of the internal conversion process within the Spx, (ii) the parallel EET from the first bright state S2 of the Spx towards the Qx state of the B890, and (iii) the internal conversion from Qx to Qy within the B890.
- Authors:
-
[1];
[2];
- Princeton Univ., NJ (United States). Dept. of Chemistry; Politecnico di Milano (Italy). Dipartimento di Fisica
- Politecnico di Milano (Italy). Dipartimento di Fisica
- Univ. of Glasgow, Scotland (United Kingdom). Glasgow Biomedical Research Centre
- Univ. of Bologna (Italy). Dipartimento di Chimica ; National Centre for Scientific Research (CNRS), Strasbourg (France)
- Madrid Institute for Advanced Studies, Madrid (Spain)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1385392
- Alternate Identifier(s):
- OSTI ID: 1228607
- Grant/Contract Number:
- SC0001035; SC 0001035
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 142; Journal Issue: 21; Related Information: PARC partners with Washington University in St. Louis (lead); University of California, Riverside; University of Glasgow, UK; Los Alamos National Laboratory; University of New Mexico; New Mexico Corsortium; North Carolina State University; Northwestern University; Oak Ridge National Laboratory; University of Pennsylvania; Sandia National Laboratories; University of Sheffield, UK; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; solar (fuels); photosynthesis (natural and artificial); biofuels (including algae and biomass); bio-inspired; charge transport; membrane; synthesis (novel materials); synthesis (self-assembly)
Citation Formats
Maiuri, Margherita, Réhault, Julien, Carey, Anne-Marie, Hacking, Kirsty, Garavelli, Marco, Lüer, Larry, Polli, Dario, Cogdell, Richard J., and Cerullo, Giulio. Ultra-broadband 2D electronic spectroscopy of carotenoid-bacteriochlorophyll interactions in the LH1 complex of a purple bacterium. United States: N. p., 2015.
Web. doi:10.1063/1.4919056.
Maiuri, Margherita, Réhault, Julien, Carey, Anne-Marie, Hacking, Kirsty, Garavelli, Marco, Lüer, Larry, Polli, Dario, Cogdell, Richard J., & Cerullo, Giulio. Ultra-broadband 2D electronic spectroscopy of carotenoid-bacteriochlorophyll interactions in the LH1 complex of a purple bacterium. United States. https://doi.org/10.1063/1.4919056
Maiuri, Margherita, Réhault, Julien, Carey, Anne-Marie, Hacking, Kirsty, Garavelli, Marco, Lüer, Larry, Polli, Dario, Cogdell, Richard J., and Cerullo, Giulio. Tue .
"Ultra-broadband 2D electronic spectroscopy of carotenoid-bacteriochlorophyll interactions in the LH1 complex of a purple bacterium". United States. https://doi.org/10.1063/1.4919056. https://www.osti.gov/servlets/purl/1385392.
@article{osti_1385392,
title = {Ultra-broadband 2D electronic spectroscopy of carotenoid-bacteriochlorophyll interactions in the LH1 complex of a purple bacterium},
author = {Maiuri, Margherita and Réhault, Julien and Carey, Anne-Marie and Hacking, Kirsty and Garavelli, Marco and Lüer, Larry and Polli, Dario and Cogdell, Richard J. and Cerullo, Giulio},
abstractNote = {We investigate the excitation energy transfer (EET) pathways in the photosynthetic light harvesting 1 (LH1) complex of purple bacterium Rhodospirillum rubrum with ultra-broadband two-dimensional electronic spectroscopy (2DES). We employ a 2DES apparatus in the partially collinear geometry, using a passive birefringent interferometer to generate the phase-locked pump pulse pair. This scheme easily lends itself to two-color operation, by coupling a sub-10 fs visible pulse with a sub-15-fs near-infrared pulse. This unique pulse combination allows us to simultaneously track with extremely high temporal resolution both the dynamics of the photoexcited carotenoid spirilloxanthin (Spx) in the visible range and the EET between the Spx and the B890 bacterio-chlorophyll (BChl), whose Qx and Qy transitions peak at 585 and 881 nm, respectively, in the near-infrared. Global analysis of the one-color and two-color 2DES maps unravels different relaxation mechanisms in the LH1 complex: (i) the initial events of the internal conversion process within the Spx, (ii) the parallel EET from the first bright state S2 of the Spx towards the Qx state of the B890, and (iii) the internal conversion from Qx to Qy within the B890.},
doi = {10.1063/1.4919056},
journal = {Journal of Chemical Physics},
number = 21,
volume = 142,
place = {United States},
year = {Tue Apr 28 00:00:00 EDT 2015},
month = {Tue Apr 28 00:00:00 EDT 2015}
}
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