Spectroscopically Orthogonal Spin Labels in Structural Biology at Physiological Temperatures

Markus Teucher; Svetlana Kucher; M. Hadi Timachi; C. Blake Wilson; Dariusz Śmiłowicz; Raphael Stoll; Nils Metzler-Nolte; Mark S. Sherwin; Songi Han; Enrica Bordignon

doi:10.1021/acs.jpcb.3c04497

Spectroscopically Orthogonal Spin Labels in Structural Biology at Physiological Temperatures

Markus Teucher, Svetlana Kucher, M. Hadi Timachi, C. Blake Wilson, Dariusz Śmiłowicz, Raphael Stoll, Nils Metzler-Nolte, Mark S. Sherwin, Songi Han, Enrica Bordignon^*

^*Corresponding author for this work

Chemistry

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

2 Scopus citations

Abstract

Electron paramagnetic resonance spectroscopy (EPR) is mostly used in structural biology in conjunction with pulsed dipolar spectroscopy (PDS) methods to monitor interspin distances in biomacromolecules at cryogenic temperatures both in vitro and in cells. In this context, spectroscopically orthogonal spin labels were shown to increase the information content that can be gained per sample. Here, we exploit the characteristic properties of gadolinium and nitroxide spin labels at physiological temperatures to study side chain dynamics via continuous wave (cw) EPR at X band, surface water dynamics via Overhauser dynamic nuclear polarization at X band and short-range distances via cw EPR at high fields. The presented approaches further increase the accessible information content on biomolecules tagged with orthogonal labels providing insights into molecular interactions and dynamic equilibria that are only revealed under physiological conditions.

Original language	English (US)
Pages (from-to)	6668-6674
Number of pages	7
Journal	Journal of Physical Chemistry B
Volume	127
Issue number	30
DOIs	https://doi.org/10.1021/acs.jpcb.3c04497
State	Published - Aug 3 2023

Funding

M.T., S.K., and E.B. thank Janine Beermann for preparing Bax and for her excellent technical assistance. This work was supported by Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany’s Excellence Strategy - EXC-2033 - Projektnummer 390677874 (EB, SH), DFG BO 3000/5-1 (EB, MT), SFB958 – Z04 (EB, MT), DFG grant INST 130/972-1 FUGG (EB) and the University of Geneva. C.B.W., S.H., and M.S.S. acknowledge support for high-field EPR work at UCSB from NSF-MCB 1617025 and 2025860. M.T., S.K., and E.B. thank Janine Beermann for preparing Bax and for her excellent technical assistance. This work was supported by Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany’s Excellence Strategy - EXC-2033 - Projektnummer 390677874 (EB, SH), DFG BO 3000/5-1 (EB, MT), SFB958 - Z04 (EB, MT), DFG grant INST 130/972-1 FUGG (EB) and the University of Geneva. C.B.W., S.H., and M.S.S. acknowledge support for high-field EPR work at UCSB from NSF-MCB 1617025 and 2025860.

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Surfaces, Coatings and Films
Materials Chemistry

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title = "Spectroscopically Orthogonal Spin Labels in Structural Biology at Physiological Temperatures",

abstract = "Electron paramagnetic resonance spectroscopy (EPR) is mostly used in structural biology in conjunction with pulsed dipolar spectroscopy (PDS) methods to monitor interspin distances in biomacromolecules at cryogenic temperatures both in vitro and in cells. In this context, spectroscopically orthogonal spin labels were shown to increase the information content that can be gained per sample. Here, we exploit the characteristic properties of gadolinium and nitroxide spin labels at physiological temperatures to study side chain dynamics via continuous wave (cw) EPR at X band, surface water dynamics via Overhauser dynamic nuclear polarization at X band and short-range distances via cw EPR at high fields. The presented approaches further increase the accessible information content on biomolecules tagged with orthogonal labels providing insights into molecular interactions and dynamic equilibria that are only revealed under physiological conditions.",

author = "Markus Teucher and Svetlana Kucher and Timachi, {M. Hadi} and Wilson, {C. Blake} and Dariusz {\'S}mi{\l}owicz and Raphael Stoll and Nils Metzler-Nolte and Sherwin, {Mark S.} and Songi Han and Enrica Bordignon",

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doi = "10.1021/acs.jpcb.3c04497",

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AU - Teucher, Markus

AU - Kucher, Svetlana

AU - Timachi, M. Hadi

AU - Wilson, C. Blake

AU - Śmiłowicz, Dariusz

AU - Stoll, Raphael

AU - Metzler-Nolte, Nils

AU - Sherwin, Mark S.

AU - Han, Songi

AU - Bordignon, Enrica

PY - 2023/8/3

Y1 - 2023/8/3

N2 - Electron paramagnetic resonance spectroscopy (EPR) is mostly used in structural biology in conjunction with pulsed dipolar spectroscopy (PDS) methods to monitor interspin distances in biomacromolecules at cryogenic temperatures both in vitro and in cells. In this context, spectroscopically orthogonal spin labels were shown to increase the information content that can be gained per sample. Here, we exploit the characteristic properties of gadolinium and nitroxide spin labels at physiological temperatures to study side chain dynamics via continuous wave (cw) EPR at X band, surface water dynamics via Overhauser dynamic nuclear polarization at X band and short-range distances via cw EPR at high fields. The presented approaches further increase the accessible information content on biomolecules tagged with orthogonal labels providing insights into molecular interactions and dynamic equilibria that are only revealed under physiological conditions.

AB - Electron paramagnetic resonance spectroscopy (EPR) is mostly used in structural biology in conjunction with pulsed dipolar spectroscopy (PDS) methods to monitor interspin distances in biomacromolecules at cryogenic temperatures both in vitro and in cells. In this context, spectroscopically orthogonal spin labels were shown to increase the information content that can be gained per sample. Here, we exploit the characteristic properties of gadolinium and nitroxide spin labels at physiological temperatures to study side chain dynamics via continuous wave (cw) EPR at X band, surface water dynamics via Overhauser dynamic nuclear polarization at X band and short-range distances via cw EPR at high fields. The presented approaches further increase the accessible information content on biomolecules tagged with orthogonal labels providing insights into molecular interactions and dynamic equilibria that are only revealed under physiological conditions.

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Spectroscopically Orthogonal Spin Labels in Structural Biology at Physiological Temperatures

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