Influence of Dy³⁺ and Tb³⁺ Doping on ¹³C Dynamic Nuclear Polarization

dc.contributor.authorNiedbalski, Peteren_US
dc.contributor.authorParish, Christopheren_US
dc.contributor.authorKiswandhi, Andhikaen_US
dc.contributor.authorFidelino, L.en_US
dc.contributor.authorKhemtong, C.en_US
dc.contributor.authorHayati, Z.en_US
dc.contributor.authorSong, L.en_US
dc.contributor.authorMartins, Andr©en_US
dc.contributor.authorSherry, A. Deanen_US
dc.contributor.authorLumata, Lloyd L.en_US
dc.contributor.utdAuthorNiedbalski, Peteren_US
dc.contributor.utdAuthorParish, Christopheren_US
dc.contributor.utdAuthorKiswandhi, Andhikaen_US
dc.contributor.utdAuthorMartins, Andr©en_US
dc.contributor.utdAuthorSherry, A. Deanen_US
dc.contributor.utdAuthorLumata, Lloyden_US
dc.description.abstractDynamic nuclear polarization (DNP) is a technique that uses a microwave-driven transfer of high spin alignment from electrons to nuclear spins. This is most effective at low temperature and high magnetic field, and with the invention of the dissolution method, the amplified nuclear magnetic resonance (NMR) signals in the frozen state in DNP can be harnessed in the liquid-state at physiologically acceptable temperature for in vitro and in vivo metabolic studies. A current optimization practice in dissolution DNP is to dope the sample with trace amounts of lanthanides such as Gd3+ or Ho3+, which further improves the polarization. While Gd³⁺ and Ho³⁺ have been optimized for use in dissolution DNP, other lanthanides have not been exhaustively studied for use in ¹³C DNP applications. In this work, two additional lanthanides with relatively high magnetic moments, Dy³⁺ and Tb³⁺, were extensively optimized and tested as doping additives for ¹³C DNP at 3.35 T and 1.2 K. We have found that both of these lanthanides are also beneficial additives, to a varying degree, for ¹³C DNP. The optimal concentrations of Dy³⁺ (1.5 mM) and Tb³⁺ (0.25 mM) for ¹³C DNP were found to be less than that of Gd³⁺ (2 mM). W-band electron paramagnetic resonance shows that these enhancements due to Dy³⁺ and Tb³⁺ doping are accompanied by shortening of electron T₁ of trityl OX063 free radical. Furthermore, when dissolution was employed, Tb³⁺-doped samples were found to have similar liquid-state ¹³C NMR signal enhancements compared to samples doped with Gd³⁺, and both Tb³⁺ and Dy³⁺ had a negligible liquid-state nuclear T₁ shortening effect which contrasts with the significant reduction in T₁ when using Gd³⁺. Our results show that Dy³⁺ doping and Tb³⁺ doping have a beneficial impact on ¹³C DNP both in the solid and liquid states, and that Tb³⁺ in particular could be used as a potential alternative to Gd³⁺ in ¹³C dissolution DNP experiments.en_US
dc.description.departmentSchool of Natural Sciences and Mathematicsen_US
dc.description.sponsorshipU.S. Department of Defense (DOD), Grant No. W81XWH-14-1-0048; Robert A.Welch Foundation, Grant Nos. AT-584 and AT-1877; NHMFL user collaboration grants program Award No. 5080; National Science Foundation (NSF) Cooperative Agreement No. DMR 1157490; National Institutes of Health (NIH) Grant No. 8P41-EB015908.en_US
dc.identifier.bibliographicCitationNiedbalski, P., C. Parish, A. Kiswandhi, L. Fidelino, et al. 2017. "Influence of Dy³⁺ and Tb³⁺ doping on ¹³C dynamic nuclear polarization." Journal of Chemical Physics 146(1), doi:10.1063/1.4973317en_US
dc.publisherAmerican Institute of Physics Incen_US
dc.rights©2017 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing.en_US
dc.sourceJournal of Chemical Physics
dc.subjectDissolution (Chemistry)en_US
dc.subjectFree radicals (Chemistry)en_US
dc.subjectMagnetic resonanceen_US
dc.subjectNuclear magnetic resonanceen_US
dc.subjectPolarization (Nuclear physics)en_US
dc.subjectRare earth metalsen_US
dc.subjectSuperconducting magnetsen_US
dc.subjectSemiconductor dopingen_US
dc.subjectRare earth metalsen_US
dc.titleInfluence of Dy³⁺ and Tb³⁺ Doping on ¹³C Dynamic Nuclear Polarizationen_US


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