TY - JOUR
T1 - Cross-Effect Dynamic Nuclear Polarization Explained
T2 - Polarization, Depolarization, and Oversaturation
AU - Equbal, Asif
AU - Leavesley, Alisa
AU - Jain, Sheetal Kumar
AU - Han, Songi
N1 - Funding Information:
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.
Funding Information:
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.
Publisher Copyright:
Copyright © 2019 American Chemical Society.
PY - 2019/2/7
Y1 - 2019/2/7
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85061147394&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85061147394&partnerID=8YFLogxK
U2 - 10.1021/acs.jpclett.8b02834
DO - 10.1021/acs.jpclett.8b02834
M3 - Article
C2 - 30645130
AN - SCOPUS:85061147394
SN - 1948-7185
VL - 10
SP - 548
EP - 558
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 3
ER -