A view of fast charge separation in the bacterial photosynthetic reaction centre involving weak environmental damping of a populated auxiliary chlorophyll state

Hammerstad-Pedersen, Jan M.; Jensen, Marianne H.; Kharkats, Yurij I.; Кузнецов, А. С.; Ulstrup, Jens

doi:10.1016/0009-2614(93)80017-j

Cited by 11 publications

(23 citation statements)

References 35 publications

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“…Excitation of P is followed by a very fast (r ~3 ps) electron transfer to the BP "primary" acceptor (whether the interposed BC plays the role of mediator in a super exchange mechanism31 or directly intervenes as an intermediate electron acceptor32 is still a subject of experimental debate). [33][34][35][36][37][38] The next step is a fast (r ~200 ps) electron transfer from BP to Q,39 followed by a slower (r ~270 ns) reduction of the oxidized P by the nearest heme group of Cy. 40 At that stage, transmembrane charge separation has been achieved with a quantum yield approaching unity (of course, only a fraction of the energy of the photon is stored as chemical energy since, Luisa De Cola was born in 1960 in Messina.…”

Section: Introductionmentioning

confidence: 99%

Ruthenium(II) and Osmium(II) Bis(terpyridine) Complexes in Covalently-Linked Multicomponent Systems: Synthesis, Electrochemical Behavior, Absorption Spectra, and Photochemical and Photophysical Properties

Sauvage¹,

Collin²,

Chambron³

et al. 1994

Chem. Rev.

1,489

1,241

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Section: Introductionmentioning

confidence: 99%

Ruthenium(II) and Osmium(II) Bis(terpyridine) Complexes in Covalently-Linked Multicomponent Systems: Synthesis, Electrochemical Behavior, Absorption Spectra, and Photochemical and Photophysical Properties

Sauvage¹,

Collin²,

Chambron³

et al. 1994

Chem. Rev.

1,489

1,241

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“…With definitions of the system coordinates (section II), energies (section III), and vertical gaps (section IV) in hand, we develop the generalization of eq 1 in section V. After describing the application to DBA systems (section VI), and some 'geometric' aspects of reaction coordinates (section VII), we close with discussion and conclusions in section VIII and summary in section IX. As in previous work, 8,12,13,14,15 we emphasize the need for a multidimensional (≥ 2) framework for treating reaction coordinates when multiple ET processes are involved.…”

Section: And Ii)mentioning

confidence: 79%

“…11 , using somewhat different notation, λ 12,13 is found for both DA and DBA systems to be positive for typical reorganization energy terms).A geometrical perspective comes from recognizing λ12,13 as an inner vector product by defining…”

mentioning

confidence: 99%

Extension of Hopfield’s Electron Transfer Model To Accommodate Site–Site Correlation

Newton

2015

J. Phys. Chem. B

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Extension of the Förster analogue for the ET rate constant (based on virtual intermediate electron detachment or attachment states) with inclusion of site-site correlation due to coulomb terms associated with solvent reorganization energy and the driving force, has been developed and illustrated for a simple three-state, two-mode model. The model is applicable to charge separation (CS), recombination (CR), and shift (CSh) ET processes, with or without an intervening bridge. The model provides a unified perspective on the role of virtual intermediate states in accounting for the thermal Franck-Condon weighted density of states (FCWD), the gaps controlling superexchange coupling, and mean absolute redox potentials, with full accommodation of site-site coulomb interactions. Two types of correlation have been analyzed: aside from the site-site correlation due to coulomb interactions, we have emphasized the intrinsic "nonorthogonality" which generally pertains to reaction coordinates (RCs) for different ET processes involving multiple electronic states, as may be expressed by suitably defined direction cosines (cos(θ)). A pair of RCs may be nonorthogonal even when the site-site coulomb correlations are absent. While different RCs are linearly independent in the mathematical sense for all θ ≠ 0°, they are independent in the sense of being "uncorrelated" only in the limit of orthogonality (θ = 90°). Application to more than two coordinates is straightforward and may include both discrete and continuum contributions.

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“…We consider from now on the diabatic limit. PBp and Phb are ß ^4^yBp', AlB ^^yHB (12) where yBp and ym are the Landau-Zener factors:…”

Section: Electronic-vibrational Coupling and Resonance In Three-cente...mentioning

confidence: 99%

Coherence, friction, and electric field effects in primary charge separation of bacterial photosynthesis.

Kharkats¹,

Кузнецов²,

Ulstrup³

1995

J. Phys. Chem.

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New electron transfer patterns have been revealed by the dynamics of the special pair chlorophyll, the auxiliary chlorophyll, and pheophytin in primary bacterial photosynthetic charge separation. We address here several of these charge transfer features for which new elements of electron transfer theory, disregarded in common theoretical approaches to photosynthetic electron transfer, are needed. These features are, first, an auxiliary chlorophyll state weakly off-resonance relative to the special pair and pheophytin states. Common superexchange views fail in this case, and incorporation of continuous vibrational manifolds in all three electronic states is essential. Secondly, external electric fields may induce transitions between the superexchange and sequential electron transfer modes where the vibrational manifolds ensure that mild resonances rather than divergence appear in the rate constant at resonance. The sequential mode finally incorporates a variety of frictional patterns ranging from vibrationally almost relaxed transitions to strongly dynamically coupled, coherent transitions.

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A view of fast charge separation in the bacterial photosynthetic reaction centre involving weak environmental damping of a populated auxiliary chlorophyll state

Cited by 11 publications

References 35 publications

Ruthenium(II) and Osmium(II) Bis(terpyridine) Complexes in Covalently-Linked Multicomponent Systems: Synthesis, Electrochemical Behavior, Absorption Spectra, and Photochemical and Photophysical Properties

Ruthenium(II) and Osmium(II) Bis(terpyridine) Complexes in Covalently-Linked Multicomponent Systems: Synthesis, Electrochemical Behavior, Absorption Spectra, and Photochemical and Photophysical Properties

Extension of Hopfield’s Electron Transfer Model To Accommodate Site–Site Correlation

Coherence, friction, and electric field effects in primary charge separation of bacterial photosynthesis.

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