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Revealing vibronic coupling in chlorophyll c1 by polarization-controlled 2D electronic spectroscopy

Bukartė, Eglė LU ; Haufe, Anja ; Paleček, David LU ; Büchel, Claudia and Zigmantas, Donatas LU orcid (2020) In Chemical Physics 530.
Abstract

Vibronic coupling between molecules has been recently discussed to play an important role in photosynthetic functions. Furthermore, this type of coupling between electronic states has been suggested to define photophysical properties of chlorophylls, a family of photosynthetic molecules. However, experimental investigation of vibronic coupling presents a major challenge. One subtle way to study vibronic coupling is by excitation and observation of superpositions of vibrational states via transitions to vibronically mixed states. Such superpositions, called coherences, are then observed as quantum beats in non-linear spectroscopy experiments. Here we present polarization-controlled two-dimensional electronic spectroscopy study of the... (More)

Vibronic coupling between molecules has been recently discussed to play an important role in photosynthetic functions. Furthermore, this type of coupling between electronic states has been suggested to define photophysical properties of chlorophylls, a family of photosynthetic molecules. However, experimental investigation of vibronic coupling presents a major challenge. One subtle way to study vibronic coupling is by excitation and observation of superpositions of vibrational states via transitions to vibronically mixed states. Such superpositions, called coherences, are then observed as quantum beats in non-linear spectroscopy experiments. Here we present polarization-controlled two-dimensional electronic spectroscopy study of the chlorophyll c1 molecule at cryogenic (77 K) temperature. By applying complex analysis to the oscillatory signals we are able to unravel vibronic coupling in this molecule. The vibronic mixing picture that we see is much more complex than was thought before.

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author
; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Chlorophyll c1, Photosynthetic pigments, Polarization-controlled multidimensional spectroscopy, Two-dimensional electronic spectroscopy, Vibronic coupling
in
Chemical Physics
volume
530
article number
110643
publisher
Elsevier
external identifiers
  • scopus:85076153777
ISSN
0301-0104
DOI
10.1016/j.chemphys.2019.110643
language
English
LU publication?
yes
id
6398f44d-7109-493c-8087-0696e647add0
date added to LUP
2021-01-13 12:14:50
date last changed
2023-11-20 20:38:12
@article{6398f44d-7109-493c-8087-0696e647add0,
  abstract     = {{<p>Vibronic coupling between molecules has been recently discussed to play an important role in photosynthetic functions. Furthermore, this type of coupling between electronic states has been suggested to define photophysical properties of chlorophylls, a family of photosynthetic molecules. However, experimental investigation of vibronic coupling presents a major challenge. One subtle way to study vibronic coupling is by excitation and observation of superpositions of vibrational states via transitions to vibronically mixed states. Such superpositions, called coherences, are then observed as quantum beats in non-linear spectroscopy experiments. Here we present polarization-controlled two-dimensional electronic spectroscopy study of the chlorophyll c1 molecule at cryogenic (77 K) temperature. By applying complex analysis to the oscillatory signals we are able to unravel vibronic coupling in this molecule. The vibronic mixing picture that we see is much more complex than was thought before.</p>}},
  author       = {{Bukartė, Eglė and Haufe, Anja and Paleček, David and Büchel, Claudia and Zigmantas, Donatas}},
  issn         = {{0301-0104}},
  keywords     = {{Chlorophyll c1; Photosynthetic pigments; Polarization-controlled multidimensional spectroscopy; Two-dimensional electronic spectroscopy; Vibronic coupling}},
  language     = {{eng}},
  publisher    = {{Elsevier}},
  series       = {{Chemical Physics}},
  title        = {{Revealing vibronic coupling in chlorophyll c1 by polarization-controlled 2D electronic spectroscopy}},
  url          = {{http://dx.doi.org/10.1016/j.chemphys.2019.110643}},
  doi          = {{10.1016/j.chemphys.2019.110643}},
  volume       = {{530}},
  year         = {{2020}},
}