From Structure to Dynamics:  Modeling Exciton Dynamics in the Photosynthetic Antenna PS1

Brüggemann, Ben; Sznee, K.E.; Novoderezhkin, Vladimir I.; Grondelle, Rienk van; May, Volkhard

doi:10.1021/jp0401473

Cited by 74 publications

(82 citation statements)

References 38 publications

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“…(19), with ω c in the order of 100 cm −1 , has been used successfully to fit the optical dynamics in photosynthetic antenna complexes. 39,40,41,42 Also, Eq. (19) without a cutoff has been used to explain the optical dynamics of aggregates of the dye 3,3'-bis(sulfopropyl)-5,5'-dichloro-9-ethylthiacarbo-cyanine (THIATS) measured between 0 and 100 K. 43 In the remainder of this paper we will use ω c = 0.2J D , which is reasonable for J-aggregates, where J D typically lies in the range 500-1000 cm The above specifies all input necessary to determine the transfer rate W k ′ A,kD [Eq.…”

Section: Resultsmentioning

confidence: 99%

Excitation Energy Transfer between Closely Spaced Multichromophoric Systems: Effects of Band Mixing and Intraband Relaxation

2006

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We theoretically analyze the excitation energy transfer between two closely spaced linear molecular J-aggregates, whose excited states are Frenkel excitons. The aggregate with the higher (lower) exciton band edge energy is considered as the donor (acceptor). The celebrated theory of Förster resonance energy transfer (FRET), which relates the transfer rate to the overlap integral of optical spectra, fails in this situation. We point out that in addition to the well-known fact that the pointdipole approximation breaks down (enabling energy transfer between optically forbidden states), also the perturbative treatment of the electronic interactions between donor and acceptor system, which underlies the Förster approach, in general loses its validity due to overlap of the exciton bands. We therefore propose a nonperturbative method, in which donor and acceptor bands are mixed and the energy transfer is described in terms of a phonon-assisted energy relaxation process between the two new (renormalized) bands. The validity of the conventional perturbative approach is investigated by comparing to the nonperturbative one; in general this validity improves for lower temperature and larger distances (weaker interactions) between the aggregates. We also demonstrate that the interference between intraband relaxation and energy transfer renders the proper definition of the transfer rate and its evaluation from experiment a complicated issue, which involves the initial excitation condition.

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Section: Resultsmentioning

confidence: 99%

Excitation Energy Transfer between Closely Spaced Multichromophoric Systems: Effects of Band Mixing and Intraband Relaxation

2006

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“…Multi-level Redfield theory was used to describe excitation energy transfer, e.g., between the strongly coupled BChls in the LH2 antenna complex (Kühn and Sundström 1997;Kühn et al 2002), in the reaction center of photosystem II (Leegwater et al 1997;Prokhorenko and Holzwarth 2000;Renger and Marcus 2002b), in the FMOprotein (Renger and May 1998;Adolphs and Renger 2006;Müh et al 2007), in photosystem I core complexes (Brüggemann et al 2004), in the LHC-II of green plants (Novoderezhkin et al 2003), in the core light-harvesting complex LH1 of purple bacteria (Novoderezhkin and van Grondelle 2002), in the WSCP complex , in the domains of strongly coupled Chls of photosystem II core complexes (Raszewski and Renger 2008), and in model dimers (Kjellberg and Pullerits 2006;Yang and Fleming 2002).…”

Section: Challenging Problems To Be Solved In the Futurementioning

confidence: 99%

Theory of excitation energy transfer: from structure to function

2009

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This mini-review summarizes our current theoretical knowledge about excitation energy transfer in pigment-protein complexes. The challenge for theory lies in the complexity of these systems and in the fact that the pigment-pigment and the pigment-protein interactions are of equal magnitude. The first part of this review contains an introduction to the theory of light harvesting and to structure- based calculations of the parameters of the theory. The second part provides a discussion of the standard Förster and Redfield theories of excitation energy transfer, which are valid in the limit of weak and strong pigment-pigment coupling, respectively. Afterward, we provide a description of recent extensions of the standard theories and discuss challenging problems to be solved in the future.

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“…In order to explain spectral and kinetic observations various modeling approaches based on the structural knowledge for Synechococcus elongatus has been performed recently (Sener et al 2002;Byrdin et al 2002;Damjanovic et al 2002;Yang et al 2003;Gobets et al 2003a, b;Bru¨ggemann et al 2004). By using full Coulomb couplings it is shown that the red spectral states can be attributed to four strongly coupled dimers (A32-B7 as C719; A33-A34 and A24-A35 as C715; B22-B34 as C708) (Sener et al 2002).…”

Section: Introductionmentioning

confidence: 99%

Red Chlorophylls in the Exciton Model of Photosystem I

Vaitekonis¹,

Trinkunas²,

Valkūnas

2005

Photosynth Res

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Structural arrangement of pigment molecules of Photosystem I of photosynthetic cyanobacterium Synechococcus elongatus is used for theoretical modeling of the excitation energy spectrum. It is demonstrated that a straightforward application of the exciton theory with the assumption of the same molecular transition energy does not describe the red side of the absorption spectrum. Since the inhomogeneity in the molecular transition energies caused by a dispersive interaction with the molecular surrounding cannot be identified directly from the structural model, the evolutionary search procedure is used for fitting the low temperature absorption and circular dichroism spectra. As a result, one dimer, three trimers and one tetramer of chlorophyll molecules responsible for the red side of the absorption spectrum with their assignment to the spectroscopically established three bands at 708, 714 and 719 nm are determined. All of them are found to be situated not in the very close vicinity of the reaction center but are encircling it almost at the same distance. In order to explain the unusual broadening on the red side of the spectrum the exciton state mixing with the charge transfer (CT) states is considered. It is shown that two effects can be distinguished as caused by mixing of those states: (i) the oscillator strength borrowing by the CT state from the exciton transition and (ii) the borrowing of the high density of the CT state by the exciton state. The intermolecular vibrations between two counter-charged molecules determine the high density in the CT state. From the broad red absorption wing it is concluded that the CT state should be the lowest state in the complexes under consideration. Such mixing effect enables resolving the diversity in the molecular transition energies as determined by different theoretical approaches.

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From Structure to Dynamics: Modeling Exciton Dynamics in the Photosynthetic Antenna PS1

Cited by 74 publications

References 38 publications

Excitation Energy Transfer between Closely Spaced Multichromophoric Systems: Effects of Band Mixing and Intraband Relaxation

Excitation Energy Transfer between Closely Spaced Multichromophoric Systems: Effects of Band Mixing and Intraband Relaxation

Theory of excitation energy transfer: from structure to function

Red Chlorophylls in the Exciton Model of Photosystem I

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