Dynamic Nuclear Polarization Using Electron Spin Cluster

Raj K. Chaklashiya; Asif Equbal; Andrey Shernyukov; Yuanxin Li; Karen Tsay; Quentin Stern; Victor Tormyshev; Elena Bagryanskaya; Songi Han

doi:10.1021/acs.jpclett.4c00182

journal article·2024-05-23Open access

Dynamic Nuclear Polarization Using Electron Spin Cluster

Raj K. Chaklashiya, Asif Equbal, Andrey Shernyukov, Yuanxin Li, Karen Tsay, Quentin Stern, Victor Tormyshev, Elena Bagryanskaya, Songi Han

The Journal of Physical Chemistry Letters· Volume 15· Issue 20

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Source abstract

Abstract

Dynamic nuclear polarization (DNP) utilizing narrow-line electron spin clusters (ESCs) to achieve nuclear spin resonance matching (ESC-DNP) by microwave irradiation is a promising way to achieve NMR signal enhancements with a wide design scope requiring low microwave power at high magnetic field. Here we present the design for a trityl-based tetra-radical (TetraTrityl) to achieve DNP for 1 H NMR at 7 T, supported by experimental data and quantum mechanical simulations. A slow-relaxing ( T 1 e ≈ 1 ms) 4-ESC is found to require at least two electron spin pairs at <8 Å e–e spin distance to yield 1 H ESC-DNP enhancement, while squeezing the rest of the e–e spin distances to <12 Å results in optimal 1 H ESC-DNP enhancements. Fast-relaxing ESCs ( T 1 e ≈ 10 μs) are found to require a weakly coupled narrow-line radical (sensitizer) to extract polarization from the ESC. These results provide design principles for achieving a power-efficient DNP at high field via ESC-DNP.

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Research context

OpenAlex topics: Advanced NMR Techniques and Applications · Atomic and Subatomic Physics Research · Quantum, superfluid, helium dynamics

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Materials Department, University of California, Santa Barbara, Santa Barbara, California 93106, United States

Division of Chemistry, New York University Abu Dhabi, Abu Dhabi, United Arab Emirates

Center for Quantum and Topological Systems, NYUAD Research Institute, New York University Abu Dhabi, PO Box 129188, Abu Dhabi, United Arab Emirates

N.N. Vorozhtsov Novosibirsk Institute of Organic Chemistry SB RAS, Novosibirsk 630090, Russia

Department of Chemistry & Biochemistry, University of California, Santa Barbara, Santa Barbara, California 93106, United States

Department of Chemistry, Northwestern University, Wilmette, Illinois 60208, United States

Department of Chemical Engineering, University of California, Santa Barbara, Santa Barbara, California 93106, United States

Funding

Division of Chemistry · Ministry of Science and Higher Education of the Russian Federation · National Institute of General Medical Sciences

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