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.

doi:10.1016/j.jmr.2023.107480

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

Journal Article · Fri May 19 00:00:00 EDT 2023 · Journal of Magnetic Resonance

DOI:https://doi.org/10.1016/j.jmr.2023.107480· OSTI ID:2421143

^[1]; Wang, Xiaoling ^[2]; Mentink-Vigier, Frédéric ^[3]; Trociewitz, Bianca ^[3]; Starck, Matthieu ^[4]; Parker, David ^[4]; Sherwin, Mark S. ^[5]; Hill, Stephen ^[6]; Krzystek, J. ^[3]

Florida State Univ., Tallahassee, FL (United States); OSTI
Florida State Univ., Tallahassee, FL (United States); Univ. of Florida, Gainesville, FL (United States); California State Univ., East Bay, Hayward, CA (United States)
Florida State Univ., Tallahassee, FL (United States)
Univ. of Durham (United Kingdom)
Univ. of California, Santa Barbara, CA (United States)
Florida State Univ., Tallahassee, FL (United States); Univ. of Florida, Gainesville, FL (United States)

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 Mn^II (3d⁵) or Gd^III (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 Gd^III complexes with potential applications as spin labels. In conclusion, 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.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Florida, Gainesville, FL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019330

OSTI ID:: 2421143

Journal Information:: Journal of Magnetic Resonance, Journal Name: Journal of Magnetic Resonance Journal Issue: C Vol. 353; ISSN 1090-7807

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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

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