Excitation Transfer in the Core Light-Harvesting Complex (LH-1) of Rhodobacter sphaeroides: An Ultrafast Fluorescence Depolarization and Annihilation Study

Bradforth, Stephen E.; Jimenez, Ralph; Mourik, Frank van; Grondelle, Rienk van; Fleming, Graham R.

doi:10.1021/j100043a071

Cited by 297 publications

(405 citation statements)

References 32 publications

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“…The power spectrum of the residual of these traces showed a clear peak at 110 cm-' due to oscillations clude that these oscillations are predominant due to wavepacket motion in the excited state. Oscillations with comparable frequency have been observed by Bradforth et al [26] in the spontaneous emission of LH1 of Rb. sphaeroides using fluorescence upconversion.…”

Section: Coherent Oscillations In Photosynthetic Antenna Systemssupporting

confidence: 69%

Photosynthetic antennae. Photosynthetic light‐harvesting

Grondelle

Monshouwer

Valkūnas

1996

Ber Bunsenges Phys Chem

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The peripheral light-harvesting complex of the photosynthetic bacterium Rhodopseudomonas acidophila (LH2) and the major plant light-harvesting complex LHCII have a very similar function: to absorb solar photons and to transfer the electronic excitation to the pigments surrounding the reaction center, the so-called 'core'. Nevertheless, their structures exhibit a dramatically different arrangement of the pigments. In LH2 the bacteriochlorophyll molecules are arranged in a highly symmetric ring, while in LHCII the positioning of the chlorophylls is very irregular. In both complexes the average distance between the pigments is 1 nm or less and, as a consequence, the electronic interaction between the pigments is strong (> 100 cm-I). Therefore, the excitation transport in these photosynthetic light-harvesting systems can not be described by a simple Fdrster type transfer mechanism, but new or other transfer mechanisms may be operative, for instance a mechanism in which the excitation is to some extent delocalized. Crucial parameters are the strength of the electronic coupling, the amount of energetic disorder and/or heterogeneity and the nature and strength of the interactions of the pigments with the protein. Here we will discuss the current status of the field of photosynthetic energy transfer in particular for LH2. We will evaluate a few simple models that contain some of the essential ingredients to describe the process of energy transfer and finally we will discuss some of the perspectives in this scientific field.

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Section: Coherent Oscillations In Photosynthetic Antenna Systemssupporting

confidence: 69%

Photosynthetic antennae. Photosynthetic light‐harvesting

Grondelle

Monshouwer

Valkūnas

1996

Ber Bunsenges Phys Chem

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“…Similar biexponential time scales are noted in spectroscopic experiments for LH2 15,18,50,51 as well as LH1. 52,53 The steady-state populations at t = 5 ps are shown in Fig. 5 along with the populations expected from Boltzmann distributed exciton states.…”

Section: A Dynamics Of a Single B850 Ringmentioning

confidence: 99%

Light harvesting complex II B850 excitation dynamics

Strümpfer¹,

Schulten²

2009

The Journal of Chemical Physics

158

258

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The dynamics of excitation energy transfer within the B850 ring of light harvesting complex 2 from Rhodobacter sphaeroides and between neighboring B850 rings is investigated by means of dissipative quantum mechanics. The assumption of Boltzmann populated donor states for the calculation of intercomplex excitation transfer rates by generalized Förster theory is shown to give accurate results since intracomplex exciton relaxation to near-Boltzmann population exciton states occurs within a few picoseconds. The primary channels of exciton transfer between B850 rings are found to be the five lowest-lying exciton states, with non-850 nm exciton states making significant contributions to the total transfer rate.

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“…This approximation was used to obtain a simple relation between time-dependent populations of exciton states, nonMarkovian optical lineshapes and pump-probe spectra. An inclusion of coherent vibrational motion found in some pigment-protein complexes [89][90][91][92][93][94] is beyond the scope of the present approach, which considers equilibrium fluctuations of the vibrations. A Markov approximation could have been used to include coherences between different exciton states.…”

Section: F Approximationsmentioning

confidence: 99%

On the relation of protein dynamics and exciton relaxation in pigment–protein complexes: An estimation of the spectral density and a theory for the calculation of optical spectra

Renger¹,

Marcus²

2002

The Journal of Chemical Physics

335

498

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A theory for calculating time-and frequency-domain optical spectra of pigment-protein complexes is presented using a density matrix approach. Non-Markovian effects in the excitonvibrational coupling are included. A correlation function is deduced from the simulation of 1.6 K fluorescence line narrowing spectra of a monomer pigment-protein complex ͑B777͒, and then used to calculate fluorescence line narrowing spectra of a dimer complex ͑B820͒. A vibrational sideband of an excitonic transition is obtained, a distinct non-Markovian feature, and agrees well with experiment on B820 complexes. The theory and the above correlation function are used elsewhere to make predictions and compare with data on time-domain pump-probe spectra and frequencydomain linear absorption, circular dichroism and fluorescence spectra of Photosystem II reaction centers.

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Excitation Transfer in the Core Light-Harvesting Complex (LH-1) of Rhodobacter sphaeroides: An Ultrafast Fluorescence Depolarization and Annihilation Study

Cited by 297 publications

References 32 publications

Photosynthetic antennae. Photosynthetic light‐harvesting

Photosynthetic antennae. Photosynthetic light‐harvesting

Light harvesting complex II B850 excitation dynamics

On the relation of protein dynamics and exciton relaxation in pigment–protein complexes: An estimation of the spectral density and a theory for the calculation of optical spectra

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