Time-domain line-shape analysis from 2D spectroscopy to precisely determine Hamiltonian parameters for a photosynthetic complex

Rolczynski, B. S. et al. (2021) Time-domain line-shape analysis from 2D spectroscopy to precisely determine Hamiltonian parameters for a photosynthetic complex. Journal of Physical Chemistry B, 125(11), pp. 2812-2820. (doi: 10.1021/acs.jpcb.0c08012) (PMID:33728918)

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Abstract

Optical signals come from coherences between quantum states, with spectral line widths determined by the coherences’ dephasing dynamics. Using a 2D electronic spectrometer, we observe weak coherence- and rephasing-time-domain signals persisting to 1 ps in the Fenna–Matthews–Olson complex at 77 K. These are coherences between the ground and excited states prepared after the complex interacts once or three times with light, rather than zero-quantum coherences that are more frequently investigated following two interactions. Here, we use these small but persistent signal components to isolate spectral contributions with narrowed peaks and reveal the system’s eigenenergies.

Item Type:Articles
Additional Information:This work was supported by the Department of Defense as part of the Vannevar Bush Fellowship (N00014-16-1-2513), the Air Force Office of Scientific Research (AFOSR FA9550-14-1-0367 and FA9550-18-1-0099), the NSF (under grant no. 1900359), and the DOE Office of Science (under award number DE-SC0020131) and the Dreyfus Foundation. S.Y., S.K., and G.S.E. were supported by the Qatar National Research Foundation exceptional grant: NPRPX-107-1-027. Additional support was provided by the Chicago MRSEC, which is funded by the NSF through Grant DMR-1420709. M.A.A. acknowledges support from an Arnold O. Beckman Postdoctoral Fellowship from the Arnold and Mabel Beckman Foundation and from a Yen Postdoctoral fellowship from the Institute for Biophysical Dynamics at The University of Chicago. R.J.C., K.A., and A.T.G. thank the Photosynthetic Antenna Research Center (PARC), an Energy Frontier Research Center funded by the Department of Energy, Office of Science, Office of Basic Energy Sciences under Award DESC0001035 for funding.
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Cogdell, Professor Richard and Gardiner, Dr Alastair and Ashraf, Mr Khuram
Authors: Rolczynski, B. S., Yeh, S.-H., Navotnaya, P., Lloyd, L. T., Ginzburg, A. R., Zheng, H., Allodi, M. A., Otto, J. P., Ashraf, K., Gardiner, A. T., Cogdell, R. J., Kais, S., and Engel, G. S.
College/School:College of Medical Veterinary and Life Sciences > Institute of Molecular Cell and Systems Biology
Journal Name:Journal of Physical Chemistry B
Publisher:American Chemical Society
ISSN:1520-6106
ISSN (Online):1520-5207
Published Online:17 March 2021
Copyright Holders:Copyright © 2021 American Chemical Society
First Published:First published in Journal of Physical Chemistry B 125(11):2812-2820
Publisher Policy:Reproduced in accordance with the publisher copyright policy

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