Tuning nuclear depolarization under MAS by electron T1e

Physical Chemistry Chemical Physics : PCCP
Alicia LundSongi Han

Abstract

The Cross-Effect (CE) Dynamic Nuclear Polarization (DNP) mechanism under Magic Angle Spinning (MAS) induces depletion or "depolarization" of the NMR signal, in the absence of microwave irradiation. In this study, the role of T1e on nuclear depolarization under MAS was tested experimentally by systematically varying the local and global electron spin concentration using mono-, bi- and tri-radicals. These spin systems show different depolarization effects that systematically tracked with their different T1e rates, consistent with theoretical predictions. In order to test whether the effect of T1e is directly or indirectly convoluted with other spin parameters, the tri-radical system was doped with different concentrations of GdCl3, only tuning the T1e rates, while keeping other parameters unchanged. Gratifyingly, the changes in the depolarization factor tracked the changes in the T1e rates. The experimental results are corroborated by quantum mechanics based numerical simulations which recapitulated the critical role of T1e. Simulations showed that the relative orientation of the two g-tensors and e-e dipolar interaction tensors of the CE fulfilling spin pair also plays a major role in determining the extent of depolarization, be...Continue Reading

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Citations

Jun 6, 2019·Chemical Communications : Chem Comm·Yuanxin LiSongi Han
Jan 31, 2020·Physical Chemistry Chemical Physics : PCCP·Frédéric Mentink-Vigier
Jun 10, 2020·Physical Chemistry Chemical Physics : PCCP·Asif EqubalSongi Han
May 11, 2019·Solid State Nuclear Magnetic Resonance·Kan TagamiSongi Han
Jan 16, 2019·The Journal of Physical Chemistry Letters·Asif EqubalSongi Han
Sep 5, 2021·Biophysical Journal·Shiying ZhuMarc-Antoine Sani

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Methods Mentioned

BETA
Nuclear Magnetic Resonance
NMR
saturation recovery

Software Mentioned

EVOLUTION
SpinEvolution
SpecMan4EPR
MAS
TOTAPOL
EasySpin
SPIN
4AT
SPINACH
MAS DNP

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