A molecular tetrad allowing efficient energy storage for 1.6 s at 163 K

Dirk M. Guldi; Hiroshi Imahori; Koichi Tamaki; Yukiyasu Kashiwagi; Hiroko Yamada; Yoshiteru Sakata; Shunichi Fukuzumi

doi:10.1021/jp036382n

A molecular tetrad allowing efficient energy storage for 1.6 s at 163 K

Dirk M. Guldi, Hiroshi Imahori, Koichi Tamaki, Yukiyasu Kashiwagi, Hiroko Yamada, Yoshiteru Sakata, Shunichi Fukuzumi

Department of Chemistry & Nanoscience

Research output: Contribution to journal › Article › peer-review

188 Scopus citations

Abstract

In a novel molecular ferrocene-zinc porphyrin-zinc porphyrin-fullerene (Fc-ZnP-ZnP-C₆₀) tetrad, the longest lifetime of a charge-separated state ever reported in an artificial photosynthetic reaction center (1.6 s n DMF at 163 K) has been attained. This lifetime is comparable, for example, to the lifetime (∼1 s) of the bacteriochlorophyll dimer radical cation ((Bchl)₂^̇+)-secondary quinone radical anion (Q_B^̇-) ion pair in the bacterial photosynthetic reaction centers. The present far distant radical ion pair is formed with a quantum yield of 34%. The radical ion pair Fc⁺-ZnP-ZnP-C₆₀^̇- produced by photoinduced electron transfer was detected by means of transient absorption spectra as well as ESR spectra. Both the lifetime and the quantum yield of the final charge-separated state are improved in Fc-ZnP-ZnP-C₆₀ relative to the corresponding ferrocene-zinc porphyrin-free base porphyrin-fullerene (Fc-ZnP-H₂P-C₆₀) tetrad.

Original language	English
Pages (from-to)	541-548
Number of pages	8
Journal	Journal of Physical Chemistry A
Volume	108
Issue number	4
DOIs	https://doi.org/10.1021/jp036382n
State	Published - 29 Jan 2004

Bibliographical note

Funding Information:
Acknowledgements. We thank Dr. Tom Hei and Dr. Roland Kanaar for providing the cell lines, support team at Brookhaven National Laboratory for helping with particle radiation, members of the Wang laboratory for helpful discussion and Doreen Theune for editing the manuscript. This work was mainly supported by grants from the National Institutes of Health (GM080771), National Aeronautics and Space Administration (NNX11AC30G, NNJ05HD36G, NNX09AU95G, NNX11AC15G and NNJ12ZSA001N) and Department of Energy (DE-AI02-10ER64969).

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@article{e2cfc7170eee42f98b9c3d0e184e6390,

title = "A molecular tetrad allowing efficient energy storage for 1.6 s at 163 K",

abstract = "In a novel molecular ferrocene-zinc porphyrin-zinc porphyrin-fullerene (Fc-ZnP-ZnP-C60) tetrad, the longest lifetime of a charge-separated state ever reported in an artificial photosynthetic reaction center (1.6 s n DMF at 163 K) has been attained. This lifetime is comparable, for example, to the lifetime (∼1 s) of the bacteriochlorophyll dimer radical cation ((Bchl){\.2}+)-secondary quinone radical anion (Q{\.B}-) ion pair in the bacterial photosynthetic reaction centers. The present far distant radical ion pair is formed with a quantum yield of 34%. The radical ion pair Fc+-ZnP-ZnP-C6{\.0}- produced by photoinduced electron transfer was detected by means of transient absorption spectra as well as ESR spectra. Both the lifetime and the quantum yield of the final charge-separated state are improved in Fc-ZnP-ZnP-C60 relative to the corresponding ferrocene-zinc porphyrin-free base porphyrin-fullerene (Fc-ZnP-H2P-C60) tetrad.",

author = "Guldi, {Dirk M.} and Hiroshi Imahori and Koichi Tamaki and Yukiyasu Kashiwagi and Hiroko Yamada and Yoshiteru Sakata and Shunichi Fukuzumi",

note = "Funding Information: Acknowledgements. We thank Dr. Tom Hei and Dr. Roland Kanaar for providing the cell lines, support team at Brookhaven National Laboratory for helping with particle radiation, members of the Wang laboratory for helpful discussion and Doreen Theune for editing the manuscript. This work was mainly supported by grants from the National Institutes of Health (GM080771), National Aeronautics and Space Administration (NNX11AC30G, NNJ05HD36G, NNX09AU95G, NNX11AC15G and NNJ12ZSA001N) and Department of Energy (DE-AI02-10ER64969).",

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AU - Tamaki, Koichi

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AU - Yamada, Hiroko

AU - Sakata, Yoshiteru

AU - Fukuzumi, Shunichi

N1 - Funding Information: Acknowledgements. We thank Dr. Tom Hei and Dr. Roland Kanaar for providing the cell lines, support team at Brookhaven National Laboratory for helping with particle radiation, members of the Wang laboratory for helpful discussion and Doreen Theune for editing the manuscript. This work was mainly supported by grants from the National Institutes of Health (GM080771), National Aeronautics and Space Administration (NNX11AC30G, NNJ05HD36G, NNX09AU95G, NNX11AC15G and NNJ12ZSA001N) and Department of Energy (DE-AI02-10ER64969).

PY - 2004/1/29

Y1 - 2004/1/29

N2 - In a novel molecular ferrocene-zinc porphyrin-zinc porphyrin-fullerene (Fc-ZnP-ZnP-C60) tetrad, the longest lifetime of a charge-separated state ever reported in an artificial photosynthetic reaction center (1.6 s n DMF at 163 K) has been attained. This lifetime is comparable, for example, to the lifetime (∼1 s) of the bacteriochlorophyll dimer radical cation ((Bchl)2̇+)-secondary quinone radical anion (QḂ-) ion pair in the bacterial photosynthetic reaction centers. The present far distant radical ion pair is formed with a quantum yield of 34%. The radical ion pair Fc+-ZnP-ZnP-C60̇- produced by photoinduced electron transfer was detected by means of transient absorption spectra as well as ESR spectra. Both the lifetime and the quantum yield of the final charge-separated state are improved in Fc-ZnP-ZnP-C60 relative to the corresponding ferrocene-zinc porphyrin-free base porphyrin-fullerene (Fc-ZnP-H2P-C60) tetrad.

AB - In a novel molecular ferrocene-zinc porphyrin-zinc porphyrin-fullerene (Fc-ZnP-ZnP-C60) tetrad, the longest lifetime of a charge-separated state ever reported in an artificial photosynthetic reaction center (1.6 s n DMF at 163 K) has been attained. This lifetime is comparable, for example, to the lifetime (∼1 s) of the bacteriochlorophyll dimer radical cation ((Bchl)2̇+)-secondary quinone radical anion (QḂ-) ion pair in the bacterial photosynthetic reaction centers. The present far distant radical ion pair is formed with a quantum yield of 34%. The radical ion pair Fc+-ZnP-ZnP-C60̇- produced by photoinduced electron transfer was detected by means of transient absorption spectra as well as ESR spectra. Both the lifetime and the quantum yield of the final charge-separated state are improved in Fc-ZnP-ZnP-C60 relative to the corresponding ferrocene-zinc porphyrin-free base porphyrin-fullerene (Fc-ZnP-H2P-C60) tetrad.

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A molecular tetrad allowing efficient energy storage for 1.6 s at 163 K

Abstract

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