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Abstract
Zero- to ultralow-field (ZULF) nuclear magnetic resonance (NMR) is an emerging tool for precision chemical analysis. In this work, we study dynamic processes and investigate the influence of chemical exchange on ZULF NMR J-spectra. We develop a computational approach that allows quantitative calculation of J-spectra in the presence of chemical exchange and apply it to study aqueous solutions of [15N]ammonium (15N\[{\mathrm{H}}_4^ +\]) as a model system. We show that pH-dependent chemical exchange substantially affects the J-spectra and, in some cases, can lead to degradation and complete disappearance of the spectral features. To demonstrate potential applications of ZULF NMR for chemistry and biomedicine, we show a ZULF NMR spectrum of [2-13C]pyruvic acid hyperpolarized via dissolution dynamic nuclear polarization (dDNP). We foresee applications of affordable and scalable ZULF NMR coupled with hyperpolarization to study chemical exchange phenomena in vivo and in situations where high-field NMR detection is not possible to implement.
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1 Department of Chemistry, University of California—Berkeley, Berkeley, CA, USA; Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA
2 Department of Chemical Engineering and Biotechnology, University of Cambridge, West Cambridge, UK; The Institute of Photonic Sciences, Castelldefels, Spain
3 Department of Radiology and Biomedical Imaging, University of California—San Francisco, San Francisco, CA, USA; Institute for Bioengineering of Catalonia, The Barcelona Institute of Science and Technology, Barcelona, Spain
4 Department of Radiology and Biomedical Imaging, University of California—San Francisco, San Francisco, CA, USA
5 Department of Chemistry, University of California—Berkeley, Berkeley, CA, USA; Food Engineering Department, Middle East Technical University, Ankara, Turkey
6 Department of Physics, University of California—Berkeley, Berkeley, CA, USA
7 Section for Biomedical Imaging, Molecular Imaging North Competence Center (MOIN CC), Department of Radiology and Neuroradiology, University Medical Center Schleswig-Holstein (UKSH), Kiel University, Kiel, Germany
8 Helmholtz-Institut Mainz, Johannes Gutenberg-Universität, Mainz, Germany
9 Department of Physics, University of California—Berkeley, Berkeley, CA, USA; Helmholtz-Institut Mainz, Johannes Gutenberg-Universität, Mainz, Germany