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Energy transfer in the major intrinsic light-harvesting complex from Amphidinium carterae

Polivka, Tomas LU ; van Stokkum, Ivo H. M. ; Zigmantas, Donatas LU orcid ; van Grondelle, Rienk ; Sundström, Villy LU and Hiller, Roger G. (2006) In Biochemistry 45(28). p.8516-8526
Abstract
Carbonyl carotenoids are important constituents of the antenna complexes of marine organisms. These carotenoids possess an excited state with a charge-transfer character ( intramolecular charge transfer state, ICT), but many details of the carotenoid to chlorophyll energy transfer mechanisms are as yet poorly understood. Here, we employ femtosecond transient absorption spectroscopy to study energy transfer pathways in the intrinsic light-harvesting complex (LHC) of dinoflagellates, which contains the carbonyl carotenoid peridinin. Carotenoid to chlorophyll energy transfer efficiency is about 90% in the 530-550 nm region, where the peridinin S-2 state transfers energy with an efficiency of 25-50%. The rest proceeds via the S-1/ICT channel,... (More)
Carbonyl carotenoids are important constituents of the antenna complexes of marine organisms. These carotenoids possess an excited state with a charge-transfer character ( intramolecular charge transfer state, ICT), but many details of the carotenoid to chlorophyll energy transfer mechanisms are as yet poorly understood. Here, we employ femtosecond transient absorption spectroscopy to study energy transfer pathways in the intrinsic light-harvesting complex (LHC) of dinoflagellates, which contains the carbonyl carotenoid peridinin. Carotenoid to chlorophyll energy transfer efficiency is about 90% in the 530-550 nm region, where the peridinin S-2 state transfers energy with an efficiency of 25-50%. The rest proceeds via the S-1/ICT channel, and the major S-1/ICT-mediated energy transfer pathway utilizes the relaxed S-1/ICT state and occurs with a time constant of 2.6 ps. Below 525 nm, the overall energy transfer efficiency drops because of light absorption by another carotenoid, diadinoxanthin, that contributes only marginally to energy transfer. Instead, its role is likely to be photoprotection. In addition to the peridinin-Chl-a energy transfer, it was shown that energy transfer also occurs between the two chlorophyll species in LHC, Chl-c(2), and Chl-a. The time constant characterizing the Chl-c2 to Chl-a energy transfer is 1.4 ps. The results demonstrate that the properties of the S1/ICT state specific for carbonyl carotenoids is the key to ensure the effective harvesting of photons in the 500-600 nm region, which is of vital importance to underwater organisms. (Less)
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author
; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Biochemistry
volume
45
issue
28
pages
8516 - 8526
publisher
The American Chemical Society (ACS)
external identifiers
  • pmid:16834325
  • wos:000238924600007
  • scopus:33746082842
ISSN
0006-2960
DOI
10.1021/bi060265b
language
English
LU publication?
yes
additional info
The information about affiliations in this record was updated in December 2015. The record was previously connected to the following departments: Chemical Physics (S) (011001060)
id
bec395ec-79b6-4065-a146-780624301102 (old id 404224)
date added to LUP
2016-04-01 12:08:38
date last changed
2021-08-18 05:30:42
@article{bec395ec-79b6-4065-a146-780624301102,
  abstract     = {Carbonyl carotenoids are important constituents of the antenna complexes of marine organisms. These carotenoids possess an excited state with a charge-transfer character ( intramolecular charge transfer state, ICT), but many details of the carotenoid to chlorophyll energy transfer mechanisms are as yet poorly understood. Here, we employ femtosecond transient absorption spectroscopy to study energy transfer pathways in the intrinsic light-harvesting complex (LHC) of dinoflagellates, which contains the carbonyl carotenoid peridinin. Carotenoid to chlorophyll energy transfer efficiency is about 90% in the 530-550 nm region, where the peridinin S-2 state transfers energy with an efficiency of 25-50%. The rest proceeds via the S-1/ICT channel, and the major S-1/ICT-mediated energy transfer pathway utilizes the relaxed S-1/ICT state and occurs with a time constant of 2.6 ps. Below 525 nm, the overall energy transfer efficiency drops because of light absorption by another carotenoid, diadinoxanthin, that contributes only marginally to energy transfer. Instead, its role is likely to be photoprotection. In addition to the peridinin-Chl-a energy transfer, it was shown that energy transfer also occurs between the two chlorophyll species in LHC, Chl-c(2), and Chl-a. The time constant characterizing the Chl-c2 to Chl-a energy transfer is 1.4 ps. The results demonstrate that the properties of the S1/ICT state specific for carbonyl carotenoids is the key to ensure the effective harvesting of photons in the 500-600 nm region, which is of vital importance to underwater organisms.},
  author       = {Polivka, Tomas and van Stokkum, Ivo H. M. and Zigmantas, Donatas and van Grondelle, Rienk and Sundström, Villy and Hiller, Roger G.},
  issn         = {0006-2960},
  language     = {eng},
  number       = {28},
  pages        = {8516--8526},
  publisher    = {The American Chemical Society (ACS)},
  series       = {Biochemistry},
  title        = {Energy transfer in the major intrinsic light-harvesting complex from Amphidinium carterae},
  url          = {http://dx.doi.org/10.1021/bi060265b},
  doi          = {10.1021/bi060265b},
  volume       = {45},
  year         = {2006},
}