Proton-Detected Solid-State NMR Spectroscopy of Spin-1/2 Nuclei with Large Chemical Shift Anisotropy

dc.contributor.author Venkatesh, Amrit
dc.contributor.author Perras, Frédéric
dc.contributor.author Rossini, Aaron
dc.contributor.department Ames Laboratory
dc.contributor.department Chemistry
dc.date 2021-06-24T19:31:29.000
dc.date.accessioned 2021-08-14T01:37:07Z
dc.date.available 2021-08-14T01:37:07Z
dc.date.embargo 2022-04-20
dc.date.issued 2021-04-20
dc.description.abstract <p>Constant-time (CT) dipolar heteronuclear multiple quantum coherence (D-HMQC) has previously been demonstrated as a method for proton detection of high-resolution wideline NMR spectra of spin-1/2 nuclei with large chemical shift anisotropy (CSA). However, 1H transverse relaxation and <em>t</em>1-noise often reduce the sensitivity of D-HMQC experiments, preventing the theoretical gains in sensitivity provided by 1H detection from being realized. Here we demonstrate a series of improved pulse sequences for 1H detection of spin-1/2 nuclei under fast MAS, with 195Pt SSNMR experiments on cisplatin as an example. First, a <em>t</em>1-incrementation protocol for D-HMQC dubbed Arbitrary Indirect Dwell (AID) is demonstrated. AID allows the use of arbitrary, rotor asynchronous <em>t</em>1-increments, but removes the constant time period from CT D-HMQC, resulting in improved sensitivity by reducing transverse relaxation losses. Next, we show that short high-power adiabatic pulses (SHAPs), which efficiently invert broad MAS sideband manifolds, can be effectively incorporated into 1H detected symmetry-based resonance echo double resonance (S-REDOR) and <em>t</em>1-noise eliminated (TONE) D-HMQC experiments. The S-REDOR experiments with SHAPs provide approximately double the dipolar dephasing, as compared to experiments with rectangular inversion pulses. We lastly show that sensitivity and resolution can be further enhanced with the use of swept excitation pulses as well as adiabatic magic angle turning (aMAT).</p>
dc.identifier archive/lib.dr.iastate.edu/ameslab_manuscripts/919/
dc.identifier.articleid 1928
dc.identifier.contextkey 23508682
dc.identifier.s3bucket isulib-bepress-aws-west
dc.identifier.submissionpath ameslab_manuscripts/919
dc.identifier.uri https://dr.lib.iastate.edu/handle/20.500.12876/aw4N4lyr
dc.language.iso en
dc.relation.ispartofseries IS-J 10476
dc.source.uri https://lib.dr.iastate.edu/cgi/viewcontent.cgi?article=2321&context=chem_pubs
dc.subject.disciplines Materials Chemistry
dc.subject.disciplines Physical Chemistry
dc.subject.keywords Structure determination
dc.subject.keywords Fast magic angle spinning
dc.subject.keywords Indirect detection
dc.subject.keywords Dipolar heteronuclear multiple quantum coherence
dc.subject.keywords D-HMQC
dc.subject.keywords REDOR
dc.subject.keywords Dipolar coupling constants
dc.title Proton-Detected Solid-State NMR Spectroscopy of Spin-1/2 Nuclei with Large Chemical Shift Anisotropy
dc.type article
dc.type.genre article
dspace.entity.type Publication
relation.isOrgUnitOfPublication 25913818-6714-4be5-89a6-f70c8facdf7e
relation.isOrgUnitOfPublication 42864f6e-7a3d-4be3-8b5a-0ae3c3830a11
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