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dc.contributor.author
Lund, Alicia
dc.contributor.author
Casano, Gilles
dc.contributor.author
Menzildjian, Georges
dc.contributor.author
Kaushik, Monu
dc.contributor.author
Stevanato, Gabriele
dc.contributor.author
Yulikov, Maxim
dc.contributor.author
Jabbour, Ribal
dc.contributor.author
Wisser, Dorothea
dc.contributor.author
Renom-Carrasco, Marc
dc.contributor.author
Thieuleux, Chloé
dc.contributor.author
Bernada, Florian
dc.contributor.author
Karoui, Hakim
dc.contributor.author
Siri, Didier
dc.contributor.author
Rosay, Melanie
dc.contributor.author
Sergeyev, Ivan V.
dc.contributor.author
Gajan, David
dc.contributor.author
Lelli, Moreno
dc.contributor.author
Emsley, Lyndon
dc.contributor.author
Ouari, Olivier
dc.contributor.author
Lesage, Anne
dc.date.accessioned
2020-03-26T12:55:36Z
dc.date.available
2020-03-25T02:33:16Z
dc.date.available
2020-03-26T12:55:36Z
dc.date.issued
2020-03-14
dc.identifier.issn
2041-6520
dc.identifier.issn
2041-6539
dc.identifier.other
10.1039/c9sc05384k
en_US
dc.identifier.uri
http://hdl.handle.net/20.500.11850/406428
dc.identifier.doi
10.3929/ethz-b-000406428
dc.description.abstract
Dynamic Nuclear Polarization (DNP) has recently emerged as a key method to increase the sensitivity of solid-state NMR spectroscopy under Magic Angle Spinning (MAS). While efficient binitroxide polarizing agents such as AMUPol have been developed for MAS DNP NMR at magnetic fields up to 9.4 T, their performance drops rapidly at higher fields due to the unfavorable field dependence of the cross-effect (CE) mechanism and AMUPol-like radicals were so far disregarded in the context of the development of polarizing agents for very high-field DNP. Here, we introduce a new family of water-soluble binitroxides, dubbed TinyPols, which have a three-bond non-conjugated flexible amine linker allowing sizable couplings between the two unpaired electrons. We show that this adjustment of the linker is crucial and leads to unexpectedly high DNP enhancement factors at 18.8 T and 21.1 T: an improvement of about a factor 2 compared to AMUPol is reported for spinning frequencies ranging from 5 to 40 kHz, with εH of up to 90 at 18.8 T and 38 at 21.1 T for the best radical in this series, which are the highest MAS DNP enhancements measured so far in aqueous solutions at these magnetic fields. This work not only breathes a new momentum into the design of binitroxides tailored towards high magnetic fields, but also is expected to push the application frontiers of high-resolution DNP MAS NMR, as demonstrated here on a hybrid mesostructured silica material.
en_US
dc.format
application/pdf
en_US
dc.language.iso
en
en_US
dc.publisher
Royal Society of Chemistry
en_US
dc.rights.uri
http://creativecommons.org/licenses/by-nc/3.0/
dc.title
TinyPols: A family of water-soluble binitroxides tailored for dynamic nuclear polarization enhanced NMR spectroscopy at 18.8 and 21.1 T
en_US
dc.type
Journal Article
dc.rights.license
Creative Commons Attribution-NonCommercial 3.0 Unported
dc.date.published
2020-02-05
ethz.journal.title
Chemical Science
ethz.journal.volume
11
en_US
ethz.journal.issue
10
en_US
ethz.journal.abbreviated
Chem. Sci.
ethz.pages.start
2810
en_US
ethz.pages.end
2818
en_US
ethz.version.deposit
publishedVersion
en_US
ethz.identifier.scopus
ethz.publication.place
Cambridge
en_US
ethz.publication.status
published
en_US
ethz.date.deposited
2020-03-25T02:34:20Z
ethz.source
SCOPUS
ethz.eth
yes
en_US
ethz.availability
Open access
en_US
ethz.rosetta.installDate
2020-03-26T12:55:47Z
ethz.rosetta.lastUpdated
2022-03-29T01:39:16Z
ethz.rosetta.versionExported
true
ethz.COinS
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