On the use of radio‐frequency offsets for ...
Type de document :
Article dans une revue scientifique: Article original
DOI :
URL permanente :
Titre :
On the use of radio‐frequency offsets for improving double‐quantum homonuclear dipolar recoupling of half‐integer‐spin quadrupolar nuclei
Auteur(s) :
Duong, Nghia Tuan [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Université Grenoble Alpes [2016-2019] [UGA [2016-2019]]
Lee, Daniel [Auteur]
Université Grenoble Alpes [2016-2019] [UGA [2016-2019]]
Mentink‐Vigier, Frédéric [Auteur]
Université Grenoble Alpes [2016-2019] [UGA [2016-2019]]
Lafon, Olivier [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
De Paëpe, Gaël [Auteur]
Université Grenoble Alpes [2016-2019] [UGA [2016-2019]]
Duong, Nghia Tuan [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Université Grenoble Alpes [2016-2019] [UGA [2016-2019]]
Lee, Daniel [Auteur]
Université Grenoble Alpes [2016-2019] [UGA [2016-2019]]
Mentink‐Vigier, Frédéric [Auteur]
Université Grenoble Alpes [2016-2019] [UGA [2016-2019]]
Lafon, Olivier [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
De Paëpe, Gaël [Auteur]
Université Grenoble Alpes [2016-2019] [UGA [2016-2019]]
Duong, Nghia Tuan [Auteur]
Titre de la revue :
Magnetic Resonance in Chemistry
Nom court de la revue :
Magn Reson Chem
Numéro :
59
Pagination :
991-1008
Date de publication :
2021-09
ISSN :
0749-1581, 1097-458X
Discipline(s) HAL :
Chimie/Chimie inorganique
Résumé en anglais : [en]
Detecting proximities between nuclei is crucial for atomic-scale structure determination with nuclear magnetic resonance (NMR) spectroscopy. Different from spin-1/2 nuclei, the methodology for quadrupolar nuclei is limited ...
Lire la suite >Detecting proximities between nuclei is crucial for atomic-scale structure determination with nuclear magnetic resonance (NMR) spectroscopy. Different from spin-1/2 nuclei, the methodology for quadrupolar nuclei is limited for solids due to the complex spin dynamics under simultaneous magic-angle spinning (MAS) and radio-frequency irradiation. Herein, the performances of several homonuclear rotary recoupling (HORROR)-based homonuclear dipolar recoupling sequences are evaluated for 27Al (spin-5/2). It is shown numerically and experimentally on mesoporous alumina that urn:x-wiley:07491581:media:mrc5142:mrc5142-math-0020 outperforms the supercycled S3 sequence and its pure double-quantum (DQ) (bracketed) version, [S3], both in terms of DQ transfer efficiency and bandwidth. This result is surprising since the S3 sequence is among the best low-power recoupling schemes for spin-1/2. The superiority of urn:x-wiley:07491581:media:mrc5142:mrc5142-math-0021 is thoroughly explained, and the crucial role of radio-frequency offsets during its spin dynamics is highlighted. The analytical approximation of urn:x-wiley:07491581:media:mrc5142:mrc5142-math-0022, derived in an offset-toggling frame, clarifies the interplay between offset and DQ efficiency, namely, the benefits of off-resonance irradiation and the trough in DQ efficiency for urn:x-wiley:07491581:media:mrc5142:mrc5142-math-0023 when the irradiation is central between two resonances, both for spin-1/2 and half-integer-spin quadrupolar nuclei. Additionally, density matrix propagations show that the urn:x-wiley:07491581:media:mrc5142:mrc5142-math-0024 sequence, applied to quadrupolar nuclei subject to quadrupolar interaction much larger than radio-frequency frequency field, can create single- and multiple-quantum coherences for near on-resonance irradiation. This significantly perturbs the creation of DQ coherences between central transitions of neighboring quadrupolar nuclei. This effect explains the DQ efficiency trough for near on-resonance irradiation, in the case of both cross-correlation and autocorrelation peaks. Overall, this work aids experimental acquisition of homonuclear dipolar correlation spectra of half-integer-spin quadrupolar nuclei and provides theoretical insights towards improving recoupling schemes at high magnetic field and fast MAS.Lire moins >
Lire la suite >Detecting proximities between nuclei is crucial for atomic-scale structure determination with nuclear magnetic resonance (NMR) spectroscopy. Different from spin-1/2 nuclei, the methodology for quadrupolar nuclei is limited for solids due to the complex spin dynamics under simultaneous magic-angle spinning (MAS) and radio-frequency irradiation. Herein, the performances of several homonuclear rotary recoupling (HORROR)-based homonuclear dipolar recoupling sequences are evaluated for 27Al (spin-5/2). It is shown numerically and experimentally on mesoporous alumina that urn:x-wiley:07491581:media:mrc5142:mrc5142-math-0020 outperforms the supercycled S3 sequence and its pure double-quantum (DQ) (bracketed) version, [S3], both in terms of DQ transfer efficiency and bandwidth. This result is surprising since the S3 sequence is among the best low-power recoupling schemes for spin-1/2. The superiority of urn:x-wiley:07491581:media:mrc5142:mrc5142-math-0021 is thoroughly explained, and the crucial role of radio-frequency offsets during its spin dynamics is highlighted. The analytical approximation of urn:x-wiley:07491581:media:mrc5142:mrc5142-math-0022, derived in an offset-toggling frame, clarifies the interplay between offset and DQ efficiency, namely, the benefits of off-resonance irradiation and the trough in DQ efficiency for urn:x-wiley:07491581:media:mrc5142:mrc5142-math-0023 when the irradiation is central between two resonances, both for spin-1/2 and half-integer-spin quadrupolar nuclei. Additionally, density matrix propagations show that the urn:x-wiley:07491581:media:mrc5142:mrc5142-math-0024 sequence, applied to quadrupolar nuclei subject to quadrupolar interaction much larger than radio-frequency frequency field, can create single- and multiple-quantum coherences for near on-resonance irradiation. This significantly perturbs the creation of DQ coherences between central transitions of neighboring quadrupolar nuclei. This effect explains the DQ efficiency trough for near on-resonance irradiation, in the case of both cross-correlation and autocorrelation peaks. Overall, this work aids experimental acquisition of homonuclear dipolar correlation spectra of half-integer-spin quadrupolar nuclei and provides theoretical insights towards improving recoupling schemes at high magnetic field and fast MAS.Lire moins >
Langue :
Anglais
Audience :
Internationale
Vulgarisation :
Non
Établissement(s) :
CNRS
Centrale Lille
ENSCL
Univ. Artois
Université de Lille
Centrale Lille
ENSCL
Univ. Artois
Université de Lille
Collections :
Équipe(s) de recherche :
RMN et matériaux inorganiques (RM2I)
Date de dépôt :
2022-03-24T09:03:00Z
2023-11-17T11:03:45Z
2023-11-17T11:03:45Z
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