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Coherence and population dynamics of chlorophyll excitations in FCP complex: Two-dimensional spectroscopy study.

Butkus, Vytautas; Gelzinis, Andrius; Augulis, Ramūnas; Gall, Andrew; Büchel, Claudia; Robert, Bruno; Zigmantas, Donatas LU ; Valkunas, Leonas and Abramavicius, Darius (2015) In Journal of Chemical Physics 142(21).
Abstract
Energy transfer processes and coherent phenomena in the fucoxanthin-chlorophyll protein complex, which is responsible for the light harvesting function in marine algae diatoms, were investigated at 77 K by using two-dimensional electronic spectroscopy. Experiments performed on femtosecond and picosecond timescales led to separation of spectral dynamics, witnessing evolutions of coherence and population states of the system in the spectral region of Qy transitions of chlorophylls a and c. Analysis of the coherence dynamics allowed us to identify chlorophyll (Chl) a and fucoxanthin intramolecular vibrations dominating over the first few picoseconds. Closer inspection of the spectral region of the Qy transition of Chl c revealed previously... (More)
Energy transfer processes and coherent phenomena in the fucoxanthin-chlorophyll protein complex, which is responsible for the light harvesting function in marine algae diatoms, were investigated at 77 K by using two-dimensional electronic spectroscopy. Experiments performed on femtosecond and picosecond timescales led to separation of spectral dynamics, witnessing evolutions of coherence and population states of the system in the spectral region of Qy transitions of chlorophylls a and c. Analysis of the coherence dynamics allowed us to identify chlorophyll (Chl) a and fucoxanthin intramolecular vibrations dominating over the first few picoseconds. Closer inspection of the spectral region of the Qy transition of Chl c revealed previously not identified, mutually non-interacting chlorophyll c states participating in femtosecond or picosecond energy transfer to the Chl a molecules. Consideration of separated coherent and incoherent dynamics allowed us to hypothesize the vibrations-assisted coherent energy transfer between Chl c and Chl a and the overall spatial arrangement of chlorophyll molecules. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Chemical Physics
volume
142
issue
21
publisher
American Institute of Physics
external identifiers
  • pmid:26049434
  • wos:000355931800018
  • scopus:84949051808
ISSN
0021-9606
DOI
10.1063/1.4914098
language
English
LU publication?
yes
id
f51543e5-65a9-489b-9e59-0ba31e1624d4 (old id 7487870)
date added to LUP
2015-07-08 11:34:23
date last changed
2017-09-03 03:09:46
@article{f51543e5-65a9-489b-9e59-0ba31e1624d4,
  abstract     = {Energy transfer processes and coherent phenomena in the fucoxanthin-chlorophyll protein complex, which is responsible for the light harvesting function in marine algae diatoms, were investigated at 77 K by using two-dimensional electronic spectroscopy. Experiments performed on femtosecond and picosecond timescales led to separation of spectral dynamics, witnessing evolutions of coherence and population states of the system in the spectral region of Qy transitions of chlorophylls a and c. Analysis of the coherence dynamics allowed us to identify chlorophyll (Chl) a and fucoxanthin intramolecular vibrations dominating over the first few picoseconds. Closer inspection of the spectral region of the Qy transition of Chl c revealed previously not identified, mutually non-interacting chlorophyll c states participating in femtosecond or picosecond energy transfer to the Chl a molecules. Consideration of separated coherent and incoherent dynamics allowed us to hypothesize the vibrations-assisted coherent energy transfer between Chl c and Chl a and the overall spatial arrangement of chlorophyll molecules.},
  articleno    = {212414},
  author       = {Butkus, Vytautas and Gelzinis, Andrius and Augulis, Ramūnas and Gall, Andrew and Büchel, Claudia and Robert, Bruno and Zigmantas, Donatas and Valkunas, Leonas and Abramavicius, Darius},
  issn         = {0021-9606},
  language     = {eng},
  number       = {21},
  publisher    = {American Institute of Physics},
  series       = {Journal of Chemical Physics},
  title        = {Coherence and population dynamics of chlorophyll excitations in FCP complex: Two-dimensional spectroscopy study.},
  url          = {http://dx.doi.org/10.1063/1.4914098},
  volume       = {142},
  year         = {2015},
}