Separating annihilation and excitation energy transfer dynamics in light harvesting systems

Mikas Vengris, Delmar S. Larsen, Leonas Valkunas, Gerdenis Kodis, Christian Herrero, John Devens Gust, Thomas A Moore, Ana L Moore, Rienk Van Grondelle

Research output: Contribution to journalArticle

8 Citations (Scopus)

Abstract

The dependence of excitation energy transfer kinetics on the electronic state of the acceptor (ground vs excited) has been resolved with a novel multipulse prePump-Pump-Probe spectroscopy. The primary energy transfer and annihilation dynamics in two model light-harvesting systems were explored: an artificially synthesized carotenoid-zinc-phthalocyanine dyad and a naturally occurring light-harvesting peridinin-chlorophyll protein complex from Amphidinium carterae. Both systems use carotenoid as the primary excitation energy donor with porphyrin chromophores as the acceptor molecules. The prePump-Pump-Probe transient signals were analyzed with Monte Carlo modeling to explicitly address the underlying step-by-step kinetics involved in both excitation migration and annihilation processes. Both energy transfer and annihilation dynamics were demonstrated to occur with approximately the same rate in both systems, regardless of the excitation status of the acceptor pigments. The possible reasons for these observations are discussed in the framework of the Förster energy transfer model.

Original languageEnglish
Pages (from-to)11372-11382
Number of pages11
JournalJournal of Physical Chemistry B
Volume117
Issue number38
DOIs
Publication statusPublished - Sep 26 2013

Fingerprint

Excitation energy
Energy transfer
energy transfer
carotenoids
Carotenoids
excitation
Pumps
Chlorophyll Binding Proteins
pumps
Kinetics
probes
Porphyrins
kinetics
Electronic states
chlorophylls
Chlorophyll
Chromophores
pigments
Pigments
porphyrins

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Materials Chemistry
  • Surfaces, Coatings and Films

Cite this

Vengris, M., Larsen, D. S., Valkunas, L., Kodis, G., Herrero, C., Gust, J. D., ... Van Grondelle, R. (2013). Separating annihilation and excitation energy transfer dynamics in light harvesting systems. Journal of Physical Chemistry B, 117(38), 11372-11382. https://doi.org/10.1021/jp403301c

Separating annihilation and excitation energy transfer dynamics in light harvesting systems. / Vengris, Mikas; Larsen, Delmar S.; Valkunas, Leonas; Kodis, Gerdenis; Herrero, Christian; Gust, John Devens; Moore, Thomas A; Moore, Ana L; Van Grondelle, Rienk.

In: Journal of Physical Chemistry B, Vol. 117, No. 38, 26.09.2013, p. 11372-11382.

Research output: Contribution to journalArticle

Vengris, Mikas ; Larsen, Delmar S. ; Valkunas, Leonas ; Kodis, Gerdenis ; Herrero, Christian ; Gust, John Devens ; Moore, Thomas A ; Moore, Ana L ; Van Grondelle, Rienk. / Separating annihilation and excitation energy transfer dynamics in light harvesting systems. In: Journal of Physical Chemistry B. 2013 ; Vol. 117, No. 38. pp. 11372-11382.
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