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Title: Exploring the Limits of Overhauser Dynamic Nuclear Polarization (O-DNP) for Portable Magnetic Resonance Detection of Low γ Nuclei

Abstract

Nuclear magnetic resonance (NMR) spectroscopy in portable, permanent magnet-based spectrometers is primarily limited to nuclei with higher gyromagnetic ratio, γ, such as 1H, 19F, and 31P due to the limited field strength achievable in these systems. Overhauser effect dynamic nuclear polarization (O-DNP), which transfers polarization from an unpaired electron to a nucleus by saturating an electron paramagnetic resonance transition with an oscillating radio frequency magnetic field, B1e, can increase the polarization of low γ nuclei by hundreds or even thousands, enabling detection in a portable system. We have investigated the potential for O-DNP to enhance signals using (4-amino-2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO hereafter) as a source of unpaired electrons in a homebuilt ultra-low field (ULF) O-DNP-NMR spectrometer. We have found, in general, that larger concentrations of TEMPO are required for effective O-DNP with low γ nuclei, which has a number of important effects. Spin exchange effects cause the EPR lines to overlap and ultimately merge at high concentrations of TEMPO, fundamentally increasing the maximum possible enhancement, while the electron–electron dipolar interaction reduces both longitudinal and transverse relaxation times for the electrons, dramatically increasing the required B1e strength. The relationship between TEMPO concentration, B1e magnitude and O-DNP enhancement is quantified, and strategies for achievingmore » these fields are discussed.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
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  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1463482
Report Number(s):
LA-UR-17-28705
Journal ID: ISSN 0937-9347; TRN: US1902304
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Applied Magnetic Resonance
Additional Journal Information:
Journal Volume: 49; Journal Issue: 7; Journal ID: ISSN 0937-9347
Country of Publication:
United States
Language:
English
Subject:
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; Atomic and Nuclear Physics; NMR Overhauser DNP ULF

Citation Formats

Yoder, Jacob Luther, Magnelind, Per Erik, Espy, Michelle A., and Janicke, Michael Timothy. Exploring the Limits of Overhauser Dynamic Nuclear Polarization (O-DNP) for Portable Magnetic Resonance Detection of Low γ Nuclei. United States: N. p., 2018. Web. doi:10.1007/s00723-018-1014-1.
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Yoder, Jacob Luther, Magnelind, Per Erik, Espy, Michelle A., & Janicke, Michael Timothy. Exploring the Limits of Overhauser Dynamic Nuclear Polarization (O-DNP) for Portable Magnetic Resonance Detection of Low γ Nuclei. United States. https://doi.org/10.1007/s00723-018-1014-1
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Yoder, Jacob Luther, Magnelind, Per Erik, Espy, Michelle A., and Janicke, Michael Timothy. Mon . "Exploring the Limits of Overhauser Dynamic Nuclear Polarization (O-DNP) for Portable Magnetic Resonance Detection of Low γ Nuclei". United States. https://doi.org/10.1007/s00723-018-1014-1. https://www.osti.gov/servlets/purl/1463482.
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@article{osti_1463482,
title = {Exploring the Limits of Overhauser Dynamic Nuclear Polarization (O-DNP) for Portable Magnetic Resonance Detection of Low γ Nuclei},
author = {Yoder, Jacob Luther and Magnelind, Per Erik and Espy, Michelle A. and Janicke, Michael Timothy},
abstractNote = {Nuclear magnetic resonance (NMR) spectroscopy in portable, permanent magnet-based spectrometers is primarily limited to nuclei with higher gyromagnetic ratio, γ, such as 1H, 19F, and 31P due to the limited field strength achievable in these systems. Overhauser effect dynamic nuclear polarization (O-DNP), which transfers polarization from an unpaired electron to a nucleus by saturating an electron paramagnetic resonance transition with an oscillating radio frequency magnetic field, B1e, can increase the polarization of low γ nuclei by hundreds or even thousands, enabling detection in a portable system. We have investigated the potential for O-DNP to enhance signals using (4-amino-2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO hereafter) as a source of unpaired electrons in a homebuilt ultra-low field (ULF) O-DNP-NMR spectrometer. We have found, in general, that larger concentrations of TEMPO are required for effective O-DNP with low γ nuclei, which has a number of important effects. Spin exchange effects cause the EPR lines to overlap and ultimately merge at high concentrations of TEMPO, fundamentally increasing the maximum possible enhancement, while the electron–electron dipolar interaction reduces both longitudinal and transverse relaxation times for the electrons, dramatically increasing the required B1e strength. The relationship between TEMPO concentration, B1e magnitude and O-DNP enhancement is quantified, and strategies for achieving these fields are discussed.},
doi = {10.1007/s00723-018-1014-1},
journal = {Applied Magnetic Resonance},
number = 7,
volume = 49,
place = {United States},
year = {2018},
month = {5}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1007/s00723-018-1014-1
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Figures / Tables:

Figure 1 Figure 1: Hardware for ULF-DNP NMR system. A) Bm magnet (large coil) and shim coils (attached to Bm magnet), side view. B) From outside to inside, Bp coils, DNP coil, and NMR solenoid, with 3 dram vial containing the sample inserted. C) Variable capacitance for tuning circuit, with DIP switchesmore » for selecting capacitors shown. This circuit is contained in an aluminum box. D) Bp coil circuit schematic. Diode and resistor prevent transmission of noise from Bp amplifier during signal detection; by giving the amplifier a negative current setting, no current can pass through the Bp coil. E) NMR tuning circuit schematic. Resistor limits current during pulses, crossed diodes prevent transmission of noise from the pulse generator from reaching the NMR coil during detection. No protection circuit for the pre-amp is needed because of the low pulse voltage because dead time is dominated by ringing rather than pre-amp recovery time. F) DNP tuning / matching circuit« less
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    Figure 7 (p. 13)figure
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