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Journal of the American Chemical Society, 2022-10, Vol.144 (39), p.18023-18029
2022
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Autor(en) / Beteiligte
Titel
Proton Hyperpolarization Relay from Nanocrystals to Liquid Water
Ist Teil von
  • Journal of the American Chemical Society, 2022-10, Vol.144 (39), p.18023-18029
Ort / Verlag
American Chemical Society
Erscheinungsjahr
2022
Quelle
Alma/SFX Local Collection
Beschreibungen/Notizen
  • Dynamic nuclear polarization (DNP) using transient electron spin polarization generated by photoexcitation can improve nuclear magnetic resonance (NMR) sensitivity far beyond the thermal equilibrium limit for analysis in life science and drug discovery. However, DNP of liquid water at room temperature remains an important challenge. Here, we propose a new method called hyperpolarization relay, in which the nonequilibrium polarization of electron spins is transferred to proton spins in the nanocrystals and then to proton spins in bulk water. Molecular nanocrystals doped with a polarizing agent that generates a highly polarized photoexcited triplet are synthesized by a reprecipitation method while controlling the size of the nanocrystals. The triplet-DNP sequence of repeated laser and microwave irradiation enhances the NMR signal of bulk water as well as nanocrystals. The smaller size of the nanocrystals increases the efficiency of polarization transfer from the nanocrystals to water due to the increased surface area. A series of control experiments and simulations based on Solomon equations confirmed the hyperpolarization relay mechanism.
Sprache
Englisch
Identifikatoren
ISSN: 0002-7863
eISSN: 1520-5126
DOI: 10.1021/jacs.2c07518
Titel-ID: cdi_proquest_miscellaneous_2715438891
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