Tailored flavoproteins acting as light-driven spin machines pump nuclear hyperpolarization

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作者
Yonghong Ding
Alexey S. Kiryutin
Ziyue Zhao
Qian-Zhao Xu
Kai-Hong Zhao
Patrick Kurle
Saskia Bannister
Tilman Kottke
Renad Z. Sagdeev
Konstantin L. Ivanov
Alexandra V. Yurkovskaya
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
来源
Scientific Reports | / 10卷
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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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