Ultrafast excited state dynamics of fucoxanthin: excitation energy dependent intramolecular charge transfer dynamics

Kosumi, Daisuke; Kusumoto, Toshiyuki; Fujii, Ritsuko; Sugisaki, Mitsuru; Iinuma, Yoshiro; Oka, Nariko; Takaesu, Yuki; Taira, Tomonori; Iha, Masahiko; Frank, Harry A.; Hashimoto, Hideki

doi:10.1039/c0cp02568b

Cited by 52 publications

(73 citation statements)

References 90 publications

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“…The species associated difference absorption spectra (SADS) show two components with lifetimes of 617 ± 20 fs and 39.0 ± 0.04 ps. This result is consistent with that of previous studies of fucoxanthin in organic solvents [46][47][48][49][50][51] . Therefore, the former component can be assigned to vibrational relaxation in the S1/ICT state of fucoxanthin and the latter component can be assigned to the internal conversion of the S1/ICT state of fucoxanthin.…”

Section: Figsupporting

confidence: 83%

“…This is a typical characteristic of the S1/ICT state of fucoxanthin. It is interesting to note that 39.0 ps lifetime is just inbetween the reported S1/ICT lifetime of fucoxanthin in methanol (23.7 ± 0.2 ps) and that in cyclohexane (62.0 ± 1.0 ps) 46 .…”

Section: Figmentioning

confidence: 91%

“…5 shows the set of time-resolved absorption spectra. Both fucoxanthin in detergent micelles and that incorporated into the LH1 complexes show a typical S1/ICT  Sn transient absorption feature that has already been described for fucoxanthin in organic solvents [44][45][46][47][48][49][50][51] . This transient absorption can be ascribed to the vibrational hot S1/ICT state and it appears immediately after excitation (see 57.6 and 307 fs spectra in Fig.…”

Section: Figmentioning

confidence: 96%

“…Details of fs pump-probe spectroscopy is described elsewhere 46,60 . The excitation pulse at 500 nm used to excite the S0 -S2 absorption band of fucoxanthin was generated by an optical parametric amplifier (Spectra Physics, OPA-800CF).…”

Section: Femtosecond Time-resolved Absorption Measurementsmentioning

confidence: 99%

“…Fucoxanthin was extracted and purified from the brown alga Cladosiphon okamuranus TOKIDA (Okinawa-Mozuku) as reported previously 46 . The purity of the fucoxanthin was confirmed to be >95% by 1 H-NMR spectroscopy.…”

Section: Isolation and Purification Of Fucoxanthinmentioning

confidence: 99%

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Strategies to enhance the excitation energy-transfer efficiency in a light-harvesting system using the intra-molecular charge transfer character of carotenoids

et al. 2017

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Strategies to enhance the excitation energy-transfer efficiency in a lightharvesting system using the intra-molecular charge transfer character of carotenoids. Faraday Discussions, 198, pp. 59-71. (doi:10.1039/c6fd00211k) This is the author's final accepted version.There may be differences between this version and the published version. You are advised to consult the publisher's version if you wish to cite from it.http://eprints.gla.ac.uk/138877/ AbstractFucoxanthin is a carotenoid that is mainly found in the light-harvesting complexes from blown algae and diatoms. Due to the presence of a carbonyl group attached to the polyene chain in polar environments excitation produces an excited intra-molecular charge transfer. This intra-molecular charge transfer state plays a key role in the highly efficient (~95%) energy-transfer from fucoxanthin to chlorophyll a in the light-harvesting complexes from brown algae. In purple bacterial lightharvesting systems the efficiency of excitation energy-transfer from carotenoids to bacteriochlorophylls depends on the extent of conjugation of the carotenoids. In this study we were successful, for the first time, to incorporate fucoxanthin into the light-harvesting complex 1 from the purple photosynthetic bacterium, Rhodospirillum rubrum G9+ (a carotenoidless strain). Femtosecond pump-probe spectroscopy was applied to this reconstituted light-harvesting complex in order to determine the efficiency of excitation energy-transfer from fucoxanthin to bacteriochlorophyll a when they are bound to the light-harvesting 1 apo-proteins.

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Section: Figsupporting

confidence: 83%

Section: Figmentioning

confidence: 91%

Section: Figmentioning

confidence: 96%

Section: Femtosecond Time-resolved Absorption Measurementsmentioning

confidence: 99%

Section: Isolation and Purification Of Fucoxanthinmentioning

confidence: 99%

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Strategies to enhance the excitation energy-transfer efficiency in a light-harvesting system using the intra-molecular charge transfer character of carotenoids

et al. 2017

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Photoelectrochemical Complexes of Fucoxanthin‐Chlorophyll Protein for Bio‐Photovoltaic Conversion with a High Open‐Circuit Photovoltage

Zhang

Cheng

Dong

et al. 2017

Chemistry An Asian Journal

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Open-circuit photovoltage (V ) is among the critical parameters for achieving an efficient light-to-charge conversion in existing solar photovoltaic devices. Natural photosynthesis exploits light-harvesting chlorophyll (Chl) protein complexes to transfer sunlight energy efficiently. We describe the exploitation of photosynthetic fucoxanthin-chlorophyll protein (FCP) complexes for realizing photoelectrochemical cells with a high V . An antenna-dependent photocurrent response and a V up to 0.72 V are observed and demonstrated in the bio-photovoltaic devices fabricated with photosynthetic FCP complexes and TiO nanostructures. Such high V is determined by fucoxanthin in FCP complexes, and is rarely found in photoelectrochemical cells with other natural light-harvesting antenna. We think that the FCP-based bio-photovoltaic conversion will provide an opportunity to fabricate environmental benign photoelectrochemical cells with high V , and also help improve the understanding of the essential physics behind the light-to-charge conversion in photosynthetic complexes.

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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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Ultrafast excited state dynamics of fucoxanthin: excitation energy dependent intramolecular charge transfer dynamics

Cited by 52 publications

References 90 publications

Strategies to enhance the excitation energy-transfer efficiency in a light-harvesting system using the intra-molecular charge transfer character of carotenoids

Strategies to enhance the excitation energy-transfer efficiency in a light-harvesting system using the intra-molecular charge transfer character of carotenoids

Photoelectrochemical Complexes of Fucoxanthin‐Chlorophyll Protein for Bio‐Photovoltaic Conversion with a High Open‐Circuit Photovoltage

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

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