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Dynamic nuclear polarization of long-lived nuclear spin states in methyl groups

Dynamic nuclear polarization of long-lived nuclear spin states in methyl groups
Dynamic nuclear polarization of long-lived nuclear spin states in methyl groups
We have induced hyperpolarized long-lived states in compounds containing 13C-bearing methyl groups by dynamic nuclear polarization (DNP) at cryogenic temperatures, followed by dissolution with a warm solvent. The hyperpolarized methyl long-lived states give rise to enhanced antiphase 13C NMR signals in solution, which often persist for times much longer than the 13C and 1H spin–lattice relaxation times under the same conditions. The DNP-induced effects are similar to quantum-rotor-induced polarization (QRIP) but are observed in a wider range of compounds because they do not depend critically on the height of the rotational barrier. We interpret our observations with a model in which nuclear Zeeman and methyl tunnelling reservoirs adopt an approximately uniform temperature, under DNP conditions. The generation of hyperpolarized NMR signals that persist for relatively long times in a range of methyl-bearing substances may be important for applications such as investigations of metabolism, enzymatic reactions, protein–ligand binding, drug screening, and molecular imaging.
1948-7185
3549-3555
Dumez, Jean-Nicolas
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Vuichoud, Basile
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Mammoli, Daniele
e70eb1c2-dab9-4de3-aa36-ffceabfe534a
Bornet, Aurélien
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Pinon, Arthur C.
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Stevanato, Gabriele
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Meier, Benno
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Bodenhausen, Geoffery
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Jannin, Sami
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Levitt, Malcolm H.
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Dumez, Jean-Nicolas
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Vuichoud, Basile
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Mammoli, Daniele
e70eb1c2-dab9-4de3-aa36-ffceabfe534a
Bornet, Aurélien
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Pinon, Arthur C.
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Stevanato, Gabriele
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Meier, Benno
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Bodenhausen, Geoffery
0ddd3782-4fda-4ca3-a056-82ec21135990
Jannin, Sami
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Levitt, Malcolm H.
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Dumez, Jean-Nicolas, Vuichoud, Basile, Mammoli, Daniele, Bornet, Aurélien, Pinon, Arthur C., Stevanato, Gabriele, Meier, Benno, Bodenhausen, Geoffery, Jannin, Sami and Levitt, Malcolm H. (2017) Dynamic nuclear polarization of long-lived nuclear spin states in methyl groups. The Journal of Physical Chemistry Letters, 8 (15), 3549-3555. (doi:10.1021/acs.jpclett.7b01512).

Record type: Article

Abstract

We have induced hyperpolarized long-lived states in compounds containing 13C-bearing methyl groups by dynamic nuclear polarization (DNP) at cryogenic temperatures, followed by dissolution with a warm solvent. The hyperpolarized methyl long-lived states give rise to enhanced antiphase 13C NMR signals in solution, which often persist for times much longer than the 13C and 1H spin–lattice relaxation times under the same conditions. The DNP-induced effects are similar to quantum-rotor-induced polarization (QRIP) but are observed in a wider range of compounds because they do not depend critically on the height of the rotational barrier. We interpret our observations with a model in which nuclear Zeeman and methyl tunnelling reservoirs adopt an approximately uniform temperature, under DNP conditions. The generation of hyperpolarized NMR signals that persist for relatively long times in a range of methyl-bearing substances may be important for applications such as investigations of metabolism, enzymatic reactions, protein–ligand binding, drug screening, and molecular imaging.

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Accepted/In Press date: 14 July 2017
e-pub ahead of print date: 19 July 2017
Published date: 3 August 2017

Identifiers

Local EPrints ID: 413351
URI: http://eprints.soton.ac.uk/id/eprint/413351
ISSN: 1948-7185
PURE UUID: 30e9507c-cefb-40c4-97de-f11fd2a0b2a5
ORCID for Benno Meier: ORCID iD orcid.org/0000-0003-2258-1507
ORCID for Malcolm H. Levitt: ORCID iD orcid.org/0000-0001-9878-1180

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Date deposited: 22 Aug 2017 16:31
Last modified: 18 Feb 2021 16:56

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Contributors

Author: Jean-Nicolas Dumez
Author: Basile Vuichoud
Author: Daniele Mammoli
Author: Aurélien Bornet
Author: Arthur C. Pinon
Author: Gabriele Stevanato
Author: Benno Meier ORCID iD
Author: Geoffery Bodenhausen
Author: Sami Jannin

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