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Tailored flavoproteins acting as light-driven spin machines pump nuclear hyperpolarization
Yonghong Ding1, Alexey S Kiryutin2,3, Ziyue Zhao1
1Institut für Analytische Chemie, Universität Leipzig, Linnéstr. 3, 04103, Leipzig, Germany.
Scientific Reports
|October 30, 2020
Summary
Researchers designed molecular spin machines to create nuclear hyperpolarization using light. This photo-chemically induced dynamic nuclear polarization (photo-CIDNP) effect enhances sensitivity in nuclear magnetic resonance (NMR) experiments.
Area of Science:
- Biophysics
- Photochemistry
- Biomolecular Engineering
Background:
- The photo-chemically induced dynamic nuclear polarization (photo-CIDNP) effect enhances nuclear magnetic resonance (NMR) sensitivity by generating non-Boltzmann nuclear spin magnetization (hyperpolarization).
- This effect is observed in photosynthetic reaction centers and modified light-oxygen-voltage (LOV) domains, where flavin mononucleotide (FMN) abstracts an electron from tryptophan to form a spin-correlated radical pair (SCRP).
Purpose of the Study:
- To engineer novel molecular spin machines capable of producing nuclear hyperpolarization upon illumination.
- To investigate the photo-CIDNP effect in designed LOV domains, including those with and without a conserved tryptophan residue.
Main Methods:
- Utilized LOV domains from Phaeodactylum tricornutum (aureochrome1a) and Methylobacterium radiotolerans (Mr4511).
- Engineered the Mr4511 LOV domain by inserting tryptophan at various positions.
- Observed photo-CIDNP effects using 15N and 1H liquid-state high-resolution NMR.
Main Results:
- Successfully generated nuclear hyperpolarization in designed molecular spin machines upon illumination.
- Observed characteristic magnetic-field dependent photo-CIDNP effects in engineered Mr4511 LOV domains.
- Evidence suggests involvement of anisotropic magnetic interactions and slow-motion dynamics in the transient paramagnetic state.
Conclusions:
- Demonstrated the successful design of molecular spin machines for light-induced nuclear hyperpolarization.
- The engineered LOV domains serve as novel systems for studying the photo-CIDNP effect.
- This biomimetic approach opens new avenues for analyzing and applying photo-CIDNP in NMR.
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