Triplet Fullerenes as Prospective Spin Labels for Nanoscale Distance Measurements by Pulsed Dipolar EPR Spectroscopy

Precise nanoscale distance measurements by pulsed electron paramagnetic resonance (EPR) spectroscopy play a crucial role in structural studies of biomolecules. The properties of the spin labels used in this approach determine the sensitivity limits, attainable distances, and proximity to biological...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2019-09, Vol.58 (38), p.13271-13275
Main Authors: Krumkacheva, Olesya A., Timofeev, Ivan O., Politanskaya, Larisa V., Polienko, Yuliya F., Tretyakov, Evgeny V., Rogozhnikova, Olga Yu, Trukhin, Dmitry V., Tormyshev, Victor M., Chubarov, Alexey S., Bagryanskaya, Elena G., Fedin, Matvey V.
Format: Article
Language:English
Subjects:
Biomolecules
Distance measurement
distance measurements
Electron paramagnetic resonance
EPR spectroscopy
Fullerenes
Hyperpolarization
Labels
Nitroxide
PELDOR
Porphyrins
Properties (attributes)
Sensitivity
Spectroscopic analysis
Spectroscopy
Spectrum analysis
spin labels
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Summary:Precise nanoscale distance measurements by pulsed electron paramagnetic resonance (EPR) spectroscopy play a crucial role in structural studies of biomolecules. The properties of the spin labels used in this approach determine the sensitivity limits, attainable distances, and proximity to biological conditions. Herein, we propose and validate the use of photoexcited fullerenes as spin labels for pulsed dipolar (PD) EPR distance measurements. Hyperpolarization and the narrower spectrum of fullerenes compared to other triplets (e.g., porphyrins) boost the sensitivity, and superior relaxation properties allow PD EPR measurements up to a near‐room temperature. This approach is demonstrated using fullerene–nitroxide and fullerene–triarylmethyl pairs, as well as a supramolecular complex of fullerene with nitroxide‐labeled protein. Photoexcited triplet fullerenes can be considered as new spin labels with outstanding spectroscopic properties for future structural studies of biomolecules. Excited and exciting: Photoexcited triplet fullerenes can be successfully used for nanoscale distance measurements in biomolecules by pulsed dipolar electron paramagnetic resonance spectroscopy. They feature outstanding spectroscopic properties as spin labels, provide drastic signal enhancement compared to all known alternatives, and are applicable up to near room temperatures.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201904152