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Title: Vibronic structure of photosynthetic pigments probed by polarized two-dimensional electronic spectroscopy and ab initio calculations

Abstract

Bacteriochlorophyll a (Bchl a) and chlorophyll a (Chl a) play important roles as light absorbers in photosynthetic antennae and participate in the initial charge-separation steps in photosynthetic reaction centers. Despite decades of study, questions remain about the interplay of electronic and vibrational states within the Q-band and its effect on the photoexcited dynamics. Here we report results of polarized two-dimensional electronic spectroscopic measurements, performed on penta-coordinated Bchl a and Chl a and their interpretation based on state-of-the-art time-dependent density functional theory calculations and vibrational mode analysis for spectral shapes. We find that the Q-band of Bchl a is comprised of two independent bands, that are assigned following the Gouterman model to Qx and Qy states with orthogonal transition dipole moments. However, we measure the angle to be ~75°, a finding that is confirmed by ab initio calculations. The internal conversion rate constant from Qx to Qy is found to be 11 ps-1. Unlike Bchl a, the Q-band of Chl a contains three distinct peaks with different polarizations. Ab initio calculations trace these features back to a spectral overlap between two electronic transitions and their vibrational replicas. The smaller energy gap and the mixing of vibronic states result in faster internalmore » conversion rate constants of 38–50 ps-1. We analyze the spectra of penta-coordinated Bchl a and Chl a to highlight the interplay between low-lying vibronic states and their relationship to photoinduced relaxation. Our findings shed new light on the photoexcited dynamics in photosynthetic systems where these chromophores are primary pigments.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [4]; ORCiD logo [1]
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  1. Department of Physics, University of Michigan, Ann Arbor, USA
  2. Department of Chemistry, University of Michigan, Ann Arbor, USA, Department of Chemistry and Biochemistry
  3. Applied Physics Program, University of Michigan, Ann Arbor, USA
  4. Department of Chemistry, University of Michigan, Ann Arbor, USA
  5. Department of Chemistry and Biochemistry, Kent State University, Kent, USA
Publication Date:
Research Org.:
Univ. of Michigan, Ann Arbor, MI (United States); Kent State Univ., Kent, OH (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1543351
Alternate Identifier(s):
OSTI ID: 1612525
Grant/Contract Number:  
SC0016384; SC0016501; CHE-1362504; CHE-1464477; CHE-1800325
Resource Type:
Published Article
Journal Name:
Chemical Science
Additional Journal Information:
Journal Name: Chemical Science Journal Volume: 10 Journal Issue: 35; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 59 BASIC BIOLOGICAL SCIENCES

Citation Formats

Song, Yin, Schubert, Alexander, Maret, Elizabeth, Burdick, Ryan K., Dunietz, Barry D., Geva, Eitan, and Ogilvie, Jennifer P. Vibronic structure of photosynthetic pigments probed by polarized two-dimensional electronic spectroscopy and ab initio calculations. United Kingdom: N. p., 2019. Web. doi:10.1039/C9SC02329A.
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Song, Yin, Schubert, Alexander, Maret, Elizabeth, Burdick, Ryan K., Dunietz, Barry D., Geva, Eitan, & Ogilvie, Jennifer P. Vibronic structure of photosynthetic pigments probed by polarized two-dimensional electronic spectroscopy and ab initio calculations. United Kingdom. doi:10.1039/C9SC02329A.
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Song, Yin, Schubert, Alexander, Maret, Elizabeth, Burdick, Ryan K., Dunietz, Barry D., Geva, Eitan, and Ogilvie, Jennifer P. Wed . "Vibronic structure of photosynthetic pigments probed by polarized two-dimensional electronic spectroscopy and ab initio calculations". United Kingdom. doi:10.1039/C9SC02329A.
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@article{osti_1543351,
title = {Vibronic structure of photosynthetic pigments probed by polarized two-dimensional electronic spectroscopy and ab initio calculations},
author = {Song, Yin and Schubert, Alexander and Maret, Elizabeth and Burdick, Ryan K. and Dunietz, Barry D. and Geva, Eitan and Ogilvie, Jennifer P.},
abstractNote = {Bacteriochlorophyll a (Bchl a) and chlorophyll a (Chl a) play important roles as light absorbers in photosynthetic antennae and participate in the initial charge-separation steps in photosynthetic reaction centers. Despite decades of study, questions remain about the interplay of electronic and vibrational states within the Q-band and its effect on the photoexcited dynamics. Here we report results of polarized two-dimensional electronic spectroscopic measurements, performed on penta-coordinated Bchl a and Chl a and their interpretation based on state-of-the-art time-dependent density functional theory calculations and vibrational mode analysis for spectral shapes. We find that the Q-band of Bchl a is comprised of two independent bands, that are assigned following the Gouterman model to Qx and Qy states with orthogonal transition dipole moments. However, we measure the angle to be ~75°, a finding that is confirmed by ab initio calculations. The internal conversion rate constant from Qx to Qy is found to be 11 ps-1. Unlike Bchl a, the Q-band of Chl a contains three distinct peaks with different polarizations. Ab initio calculations trace these features back to a spectral overlap between two electronic transitions and their vibrational replicas. The smaller energy gap and the mixing of vibronic states result in faster internal conversion rate constants of 38–50 ps-1. We analyze the spectra of penta-coordinated Bchl a and Chl a to highlight the interplay between low-lying vibronic states and their relationship to photoinduced relaxation. Our findings shed new light on the photoexcited dynamics in photosynthetic systems where these chromophores are primary pigments.},
doi = {10.1039/C9SC02329A},
journal = {Chemical Science},
number = 35,
volume = 10,
place = {United Kingdom},
year = {2019},
month = {9}
}
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DOI: 10.1039/C9SC02329A
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