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

Song, Yin; Schubert, Alexander; Maret, Elizabeth; Burdick, Ryan K.; Dunietz, Barry D.; Geva, Eitan; Ogilvie, Jennifer P.

doi:10.1039/c9sc02329a

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

Journal Article · 03 July 2019 · Chemical Science

DOI: https://doi.org/10.1039/c9sc02329a · OSTI ID:1543351

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Univ. of Michigan, Ann Arbor, MI (United States)
Univ. of Michigan, Ann Arbor, MI (United States); Kent State Univ., Kent, OH (United States)
Kent State Univ., Kent, OH (United States)

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 Q_x and Q_y 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 Q_x to Q_y 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.

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Research Organization:: Univ. of Michigan, Ann Arbor, MI (United States); Kent State Univ., Kent, OH (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0016384; SC0016501; CHE-1362504; CHE-1464477; CHE-1800325

OSTI ID:: 1543351

Alternate ID(s):: OSTI ID: 1612525; OSTI ID: 1773847

Journal Information:: Chemical Science, Vol. 10, Issue 35; ISSN 2041-6520

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 38 works

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