Pulsed dynamic nuclear polarization (DNP) enhances the nuclear magnetic resonance sensitivity by coherently transferring electron spin polarization to dipolar coupled nuclear spins. Recently, many new pulsed DNP techniques such as NOVEL, TOP, XiX, TPPM, and BEAM have been introduced. Despite significant progress, numerous challenges remain unsolved. The electron-electron (e-e) interactions in these sequences can severely disrupt the efficiency of electron-nuclear (e-n) polarization transfer. In order to tackle this issue, we propose the magic-NOVEL DNP method, utilizing Lee-Goldburg decoupling to counteract e-e coupling effects. Our theoretical analysis and quantum mechanical simulations reveal that magic-NOVEL significantly improves the transfer efficiency of DNP, even at shorter e-e distances. This method offers a new perspective for advancing pulsed DNP techniques in systems with dense electron spin baths. Furthermore, we demonstrate the effectiveness of phase-modulated Lee-Goldburg sequences in improving pulsed DNP transfer.
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http://dx.doi.org/10.1063/5.0241288 | DOI Listing |
J Clin Med
December 2024
Cardiovascular Pathophysiology and Genomics Research Unit, School of Physiology, Faculty of Health Sciences, University of the Witwatersrand, Johannesburg 2193, South Africa.
The study aimed to assess the potential impacts of mean arterial pressure (MAP) and its determinants (cardiac output and systemic vascular resistance) on diabetic nephropathy (DNP)-associated impaired aortic function. This multi-ethnic study included 115 chronic kidney disease (CKD) patients (67 non-dialysis and 48 dialysis). Six aortic function measures were evaluated by SpygmoCor.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Center for Quantum and Topological Systems, New York University Abu Dhabi, P.O. Box 129188, Abu Dhabi, United Arab Emirates.
Pulsed dynamic nuclear polarization (DNP) enhances the nuclear magnetic resonance sensitivity by coherently transferring electron spin polarization to dipolar coupled nuclear spins. Recently, many new pulsed DNP techniques such as NOVEL, TOP, XiX, TPPM, and BEAM have been introduced. Despite significant progress, numerous challenges remain unsolved.
View Article and Find Full Text PDFPhys Chem Chem Phys
November 2024
Interdisciplinary Nanoscience Center (iNANO) and Department of Chemistry, Aarhus University, Gustav Wieds Vej 14, DK-8000 Aarhus C, Denmark.
Dynamic nuclear polarization (DNP) has proven to be a powerful technique to enhance nuclear spin polarization by transferring the much higher electron spin polarization to nuclear spins prior to detection. While major attention has been devoted to high-field applications with continuous microwave irradiation, the introduction of fast arbitrary waveform generators is gradually increasing opportunities for the realization of pulsed DNP. Here, we describe how static-powder DNP pulse sequences may systematically be designed using single-spin vector effective Hamiltonian theory.
View Article and Find Full Text PDFSci Adv
October 2024
Interdisciplinary Nanoscience Center (iNANO) and Department of Chemistry, Aarhus University, Gustav Wieds Vej 14, DK-8000 Aarhus C, Denmark.
It is demonstrated that the time evolution of the electron-nuclear polarization transfer process during pulsed dynamic nuclear polarization (DNP) can be reversed on a microsecond timescale, leading to the observation of DNP echoes. The DNP echoes are induced by consecutive application of two pulse trains that produce effective Hamiltonians that differ only in the sign of the effective hyperfine coupling. The experiments have been performed on a frozen solution of trityl radicals in water/glycerol on a homebuilt X-band electron paramagnetic resonance/DNP spectrometer at 80 kelvins.
View Article and Find Full Text PDFJ Magn Reson
November 2024
Laboratory of Chemical Physics, National Institute of Diabetes and Digestive and Kidney Diseases, National Institutes of Health, Bethesda, MD 20892-0520, U.S.A. Electronic address:
Dynamic nuclear polarization (DNP) enhanced magic angle spinning (MAS) solid-state NMR carried out at 25 K enables rapid acquisition of multi-dimensional C-N correlation spectra for protein structure studies and resonance assignment. Under commonly used DNP conditions, solvent deuteration reduces H-N cross polarization (CP) efficiencies, necessitates more careful optimization, and requires longer high-power N radio-frequency pulses. The sensitivity of 2D heteronuclear correlation experiments is potentially impaired.
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