Tailored flavoproteins acting as light-driven spin machines pump nuclear hyperpolarization
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作者:
Yonghong Ding
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机构:Universität Leipzig,Institut für Analytische Chemie
Yonghong Ding
Alexey S. Kiryutin
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机构:Universität Leipzig,Institut für Analytische Chemie
Alexey S. Kiryutin
Ziyue Zhao
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机构:Universität Leipzig,Institut für Analytische Chemie
Ziyue Zhao
Qian-Zhao Xu
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机构:Universität Leipzig,Institut für Analytische Chemie
Qian-Zhao Xu
Kai-Hong Zhao
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机构:Universität Leipzig,Institut für Analytische Chemie
Kai-Hong Zhao
Patrick Kurle
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机构:Universität Leipzig,Institut für Analytische Chemie
Patrick Kurle
Saskia Bannister
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机构:Universität Leipzig,Institut für Analytische Chemie
Saskia Bannister
Tilman Kottke
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机构:Universität Leipzig,Institut für Analytische Chemie
Tilman Kottke
Renad Z. Sagdeev
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机构:Universität Leipzig,Institut für Analytische Chemie
Renad Z. Sagdeev
Konstantin L. Ivanov
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机构:Universität Leipzig,Institut für Analytische Chemie
Konstantin L. Ivanov
Alexandra V. Yurkovskaya
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机构:Universität Leipzig,Institut für Analytische Chemie
Alexandra V. Yurkovskaya
Jörg Matysik
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机构:Universität Leipzig,Institut für Analytische Chemie
Jörg Matysik
机构:
[1] Universität Leipzig,Institut für Analytische Chemie
[2] Siberian Branch of Russian Academy of Sciences,International Tomography Center
[3] Novosibirsk State University,State Key Laboratory of Agricultural Microbiology
[4] Huazhong Agricultural University,Physikalische und Biophysikalische Chemie
[5] Universität Bielefeld,undefined
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Scientific Reports
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摘要:
The solid-state photo-chemically induced dynamic nuclear polarization (photo-CIDNP) effect generates non-Boltzmann nuclear spin magnetization, referred to as hyperpolarization, allowing for high gain of sensitivity in nuclear magnetic resonance (NMR). Well known to occur in photosynthetic reaction centers, the effect was also observed in a light-oxygen-voltage (LOV) domain of the blue-light receptor phototropin, in which the functional cysteine was removed to prevent photo-chemical reactions with the cofactor, a flavin mononucleotide (FMN). Upon illumination, the FMN abstracts an electron from a tryptophan to form a transient spin-correlated radical pair (SCRP) generating the photo-CIDNP effect. Here, we report on designed molecular spin-machines producing nuclear hyperpolarization upon illumination: a LOV domain of aureochrome1a from Phaeodactylum tricornutum, and a LOV domain named 4511 from Methylobacterium radiotolerans (Mr4511) which lacks an otherwise conserved tryptophan in its wild-type form. Insertion of the tryptophan at canonical and novel positions in Mr4511 yields photo-CIDNP effects observed by 15N and 1H liquid-state high-resolution NMR with a characteristic magnetic-field dependence indicating an involvement of anisotropic magnetic interactions and a slow-motion regime in the transient paramagnetic state. The heuristic biomimetic design opens new categories of experiments to analyze and apply the photo-CIDNP effect.
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Penn State Univ, Dept Engn Sci & Mech, University Pk, PA 16802 USAPenn State Univ, Dept Engn Sci & Mech, University Pk, PA 16802 USA
Zheng, Yue Bing
Hao, Qingzhen
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Penn State Univ, Dept Engn Sci & Mech, University Pk, PA 16802 USA
Penn State Univ, Dept Phys, University Pk, PA 16802 USAPenn State Univ, Dept Engn Sci & Mech, University Pk, PA 16802 USA
Hao, Qingzhen
Yang, Ying-Wei
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Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USAPenn State Univ, Dept Engn Sci & Mech, University Pk, PA 16802 USA
Yang, Ying-Wei
Kiraly, Brian
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Penn State Univ, Dept Engn Sci & Mech, University Pk, PA 16802 USAPenn State Univ, Dept Engn Sci & Mech, University Pk, PA 16802 USA
Kiraly, Brian
Chiang, I-Kao
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Penn State Univ, Dept Engn Sci & Mech, University Pk, PA 16802 USAPenn State Univ, Dept Engn Sci & Mech, University Pk, PA 16802 USA
Chiang, I-Kao
Huang, Tony Jun
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Penn State Univ, Dept Engn Sci & Mech, University Pk, PA 16802 USAPenn State Univ, Dept Engn Sci & Mech, University Pk, PA 16802 USA
机构:
Nagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, Japan
Nagoya Inst Technol, OptoBioTechnol Res Ctr, Showa Ku, Nagoya, Aichi 4668555, Japan
Japan Sci & Technol Agcy, PRESTO, 4-1-8 Honcho, Kawaguchi, Saitama 3320012, JapanNagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, Japan
Inoue, Keiichi
Ito, Shota
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Nagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, JapanNagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, Japan
Ito, Shota
Kato, Yoshitaka
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Nagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, JapanNagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, Japan
Kato, Yoshitaka
Nomura, Yurika
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Nagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, JapanNagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, Japan
Nomura, Yurika
Shibata, Mikihiro
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Kanazawa Univ, Dept Phys, Kanazawa, Ishikawa 9201192, Japan
Kanazawa Univ, BioAFM Frontier Res Ctr, Kanazawa, Ishikawa 9201192, JapanNagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, Japan
Shibata, Mikihiro
Uchihashi, Takayuki
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Kanazawa Univ, Dept Phys, Kanazawa, Ishikawa 9201192, Japan
Kanazawa Univ, BioAFM Frontier Res Ctr, Kanazawa, Ishikawa 9201192, JapanNagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, Japan
Uchihashi, Takayuki
Tsunoda, Satoshi P.
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Nagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, JapanNagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, Japan
Tsunoda, Satoshi P.
Kandori, Hideki
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机构:
Nagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, Japan
Nagoya Inst Technol, OptoBioTechnol Res Ctr, Showa Ku, Nagoya, Aichi 4668555, JapanNagoya Inst Technol, Dept Life Sci & Appl Chem, Showa Ku, Nagoya, Aichi 4668555, Japan