Cross-Effect Dynamic Nuclear Polarization Explained: Polarization, Depolarization, and Oversaturation

Asif Equbal, Alisa Leavesley, Sheetal Kumar Jain, Songi Han*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

30 Scopus citations

Abstract

The scope of this Perspective is to analytically describe NMR hyperpolarization by the three-spin cross effect (CE) dynamic nuclear polarization (DNP) using an effective Hamiltonian concept. We apply, for the first time, the bimodal operator-based Floquet theory in the Zeeman-interaction frame for two and three coupled spins to derive the known interaction Hamiltonian for CE-DNP. With a unified understanding of CE-DNP, and supported by empirical observation of the state of electron spin polarization under the given experimental conditions, we explain diverse manifestations of CE from oversaturation, enhanced hyperpolarization by broad-band saturation, to nuclear spin depolarization under magic-angle spinning.

Original languageEnglish (US)
Pages (from-to)548-558
Number of pages11
JournalJournal of Physical Chemistry Letters
Volume10
Issue number3
DOIs
StatePublished - Feb 7 2019

Funding

We thank Yuanxin Li for fruitful discussion on CE-DNP. This work was supported by the National Science Foundation (CHE #1505038 to S.H.), the National Institute of Health (NIBIB #1R21EB022731 and #R21GM103477 to S.H.), and Binational Science Foundation (Grant #2014149 to S.H.). The content is solely the responsibility of the authors and does not necessarily represent the official views of the National Institutes of Health. Songi Han received her Doctoral Degree in Natural Sciences (Dr.rer.nat) from Aachen University of Technology (RWTH), Germany, in 2001. She pursued her postdoctoral studies at the University of California Berkeley sponsored by the Feodor Lynen Fellowship of the Alexander von Humboldt Foundation. Dr. Han joined the faculty at University of California Santa Barbara (UCSB) in 2004, received tenure in 2010, and was promoted to full professor in 2012. She is currently a Professor in the Department of Chemistry and Biochemistry and the Department of Chemical Engineering at UCSB. She is a recipient of the 2008 Packard Fellowship for Science and Engineering, the 2010 Dreyfus-Teacher Scholar Award, the 2011 NIH Innovator Award, the 2015 Bessel Prize of the Alexander von Humboldt Foundation, and the 2018 recipient of the Biophysical Society Innovator Award. Her research group focuses on mechanistic studies of DNP as well as broadening the application scope of DNP and EPR.

ASJC Scopus subject areas

  • General Materials Science
  • Physical and Theoretical Chemistry

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