Ultrafast Energy‐Transfer Pathway in a Purple‐Bacterial Photosynthetic Core Antenna, as Revealed by Femtosecond Time‐Resolved Spectroscopy

Kosumi, Daisuke; Maruta, Satoshi; Horibe, Tomoko; Fujii, Ritsuko; Sugisaki, Mitsuru; Cogdell, Richard J.; Hashimoto, Hideki

doi:10.1002/anie.201003771

Cited by 29 publications

(16 citation statements)

References 18 publications

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“…This supports the presence of the reverse pathway of Bchl → Car EET in Rsp. rubrum S1 19. In contrast, the temporal profile of the absorbance changes of Rba.…”

Section: Resultsmentioning

confidence: 92%

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The dependence of excitation energy transfer pathways on conjugation length of carotenoids in purple bacterial photosynthetic antennae

Maruta

Kosumi

Horibe

et al. 2010

Physica Status Solidi (b)

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Phone: þ81 6 6605 3627, Fax: þ81 6 6605 3619Ultrafast excited state dynamics of carotenoids in solution and bound to pigment-protein complexes have been investigated by femtosecond pump-probe spectroscopic measurements. Possible excitation energy transfer (EET) pathways between carotenoids and bacteriochlorophylls and their efficiency depend strongly on the conjugation length of carotenoids. In the case of Rhodobacter sphaeroides 2.4.1, dual EET channels from carotenoid to bacteriochlorophyll (S 2 ! Q x and S 1 ! Q y ) upon excitation of carotenoid were observed. In the case of Rhodospirillum rubrum S1, on the other hand, the EET pathway of S 1 ! Q y upon excitation of carotenoid was closed, whereas reverse energy transfer from bacteriochlorophyll to carotenoid was clearly observed upon excitation of bacteriochlorophyll. The role of carotenoids in the light-harvesting complexes is discussed in terms of their conjugation length.

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“…This supports the presence of the reverse pathway of Bchl → Car EET in Rsp. rubrum S1 19. In contrast, the temporal profile of the absorbance changes of Rba.…”

Section: Resultsmentioning

confidence: 92%

“…The appearance of the S 1 signal of Spx after excitation to Q x suggests the involvement of reverse Bchl → Car EET in Rsp. rubrum S1 19.…”

Section: Resultsmentioning

confidence: 99%

The dependence of excitation energy transfer pathways on conjugation length of carotenoids in purple bacterial photosynthetic antennae

Maruta

Kosumi

Horibe

et al. 2010

Physica Status Solidi (b)

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“…rubrum chromatophores, which were interpreted to show the possibility of reverse EET from BChl Q x to Cars. 32 However, to assume that this may be a universal mechanism is not necessarily warranted, since no measurements have been made so far with LHCs from other (purple) bacteria. Perhaps, this effect is a consequence of specific features of the structure of the photosynthetic apparatus of Rps.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Lack of Excitation Energy Transfer from the Bacteriochlorophyll Soret Band to Carotenoids in Photosynthetic Complexes of Purple Bacteria

et al. 2021

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The excitation energy transfer (EET) from the bacteriochlorophyll (BChl) Soret band to the second excited state(s) (S2) of carotenoids in pigment–protein complexes of purple bacteria was investigated. The efficiency of EET was determined, based on fluorescence excitation and absorption spectra of chromatophores, peripheral light-harvesting complexes (LH2), core complexes (LH1-RC), and pigments in solution. Carotenoid-containing and carotenoid-less samples were compared: LH1-RC and LH2 from Allochromatium minutissimum, Ectothiorhodospira haloalkaliphila, and chromatophores from Rhodobacter sphaeroides and Rhodospirillum rubrum wild type and carotenoid-free strains R-26 and G9. BChl-to-carotenoid EET was absent, or its efficiency was less than the accuracy of the measurements of ∼5%. Quantum chemical calculations support the experimental results: The transition dipole moments of spatially close carotenoid/BChl pairs were found to be nearly orthogonal. The structural arrangements suggest that Soret EET may be lacking for the studied systems, however, EET from carotenoids to Q x appears to be possible.

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“…rubrum S1 was reported based on femtosecond time-resolved spectroscopy. [359] This energy transfer occurs from the Q x state of the BChl to the S 1 state of the carotenoid. It was shown that a major contribution (40 %) of the energy initially transferred from the S 2 state of the carotenoid to the Q x state in the BChl is returned back to the carotenoid (S 1 ).…”

Section: Role Of the Carotenoidsmentioning

confidence: 99%

Quantum Chemical Description of Absorption Properties and Excited‐State Processes in Photosynthetic Systems

2011

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The theoretical description of the initial steps in photosynthesis has gained increasing importance over the past few years. This is caused by more and more structural data becoming available for light-harvesting complexes and reaction centers which form the basis for atomistic calculations and by the progress made in the development of first-principles methods for excited electronic states of large molecules. In this Review, we discuss the advantages and pitfalls of theoretical methods applicable to photosynthetic pigments. Besides methodological aspects of excited-state electronic-structure methods, studies on chlorophyll-type and carotenoid-like molecules are discussed. We also address the concepts of exciton coupling and excitation-energy transfer (EET) and compare the different theoretical methods for the calculation of EET coupling constants. Applications to photosynthetic light-harvesting complexes and reaction centers based on such models are also analyzed.

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Ultrafast Energy‐Transfer Pathway in a Purple‐Bacterial Photosynthetic Core Antenna, as Revealed by Femtosecond Time‐Resolved Spectroscopy

Cited by 29 publications

References 18 publications

The dependence of excitation energy transfer pathways on conjugation length of carotenoids in purple bacterial photosynthetic antennae

The dependence of excitation energy transfer pathways on conjugation length of carotenoids in purple bacterial photosynthetic antennae

Lack of Excitation Energy Transfer from the Bacteriochlorophyll Soret Band to Carotenoids in Photosynthetic Complexes of Purple Bacteria

Quantum Chemical Description of Absorption Properties and Excited‐State Processes in Photosynthetic Systems

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