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Terahertz EPR spectroscopy using a 36-tesla high-homogeneity series-connected hybrid magnet

Dubroca, Thierry; Wang, Xiaoling; Mentink-Vigier, Frédéric; Trociewitz, Bianca; Starck, Matthieu; Parker, David; Sherwin, Mark S.; Hill, Stephen; Krzystek, J.

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Authors

Thierry Dubroca

Xiaoling Wang

Frédéric Mentink-Vigier

Bianca Trociewitz

Mark S. Sherwin

Stephen Hill

J. Krzystek



Abstract

Electron Paramagnetic Resonance (EPR) is a powerful technique to study materials and biological samples on an atomic scale. High-field EPR in particular enables extracting very small g-anisotropies in organic radicals and half-filled 3d and 4f metal ions such as MnII (3d5) or GdIII (4f7), and resolving EPR signals from unpaired spins with very close g-values, both of which provide high-resolution details of the local atomic environment. Before the recent commissioning of the high-homogeneity Series Connected Hybrid magnet (SCH, superconducting + resistive) at the National High Magnetic Field Laboratory (NHMFL), the highest-field, high-resolution EPR spectrometer available was limited to 25 T using a purely resistive “Keck” magnet at the NHMFL. Herein, we report the first EPR experiments performed using the SCH magnet capable of reaching the field of 36 T, corresponding to an EPR frequency of 1 THz for g = 2. The magnet’s intrinsic homogeneity (25 ppm, that is 0.9 mT at 36 T over 1 cm diameter, 1 cm length cylinder) was previously established by NMR. We characterized the magnet’s temporal stability (5 ppm, which is 0.2 mT at 36 T over one-minute, the typical acquisition time) using 2,2-diphenyl-1-picrylhydrazyl (DPPH). This high resolution enables resolving the weak g-anisotropy of 1,3-bis(diphenylene)-2-phenylallyl (BDPA), Δg = 2.5 × 10–4 obtained from measurements at 932 GHz and 33 T. Subsequently, we recorded EPR spectra at multiple frequencies for two GdIII complexes with potential applications as spin labels. We demonstrated a significant reduction in line broadening in Gd[DTPA], attributed to second order zero field splitting, and a resolution enhancement of g-tensor anisotropy for Gd[sTPATCN]-SL.

Citation

Dubroca, T., Wang, X., Mentink-Vigier, F., Trociewitz, B., Starck, M., Parker, D., Sherwin, M. S., Hill, S., & Krzystek, J. (2023). Terahertz EPR spectroscopy using a 36-tesla high-homogeneity series-connected hybrid magnet. Journal of Magnetic Resonance, 353, Article 107480. https://doi.org/10.1016/j.jmr.2023.107480

Journal Article Type Article
Acceptance Date May 13, 2023
Online Publication Date May 19, 2023
Publication Date 2023-08
Deposit Date Dec 19, 2023
Publicly Available Date May 20, 2024
Journal Journal of Magnetic Resonance
Print ISSN 1090-7807
Publisher Elsevier
Peer Reviewed Peer Reviewed
Volume 353
Article Number 107480
DOI https://doi.org/10.1016/j.jmr.2023.107480
Public URL https://durham-repository.worktribe.com/output/2047571

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