期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 21, 期 5, 页码 2595-2600出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8cp06883f
关键词
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资金
- NSF [CHE-1412568, CHE-1710046]
- Diamond Jubilee Visiting Fellowship
- NSF REU grant (REU in Chemical Biology at NYU)
- National Science Foundation [CHE-01162222]
The examination and optimized preparation of nuclear spin singlet order has enabled the development of new types of applications that rely on potentially long-term polarization storage. Lifetimes several orders of magnitude longer than T-1 have been observed. The efficient creation of such states relies on special pulse sequences. The extreme cases of very large and very small magnetic equivalence received primary attention, while relatively little effort has been directed towards studying singlet relaxation in the intermediate regime. The intermediate case is of interest as it is relevant for many spin systems, and would also apply to heteronuclear systems in very low magnetic fields. Experimental evidence for singlet-triplet leakage in the intermediate regime is sparse. Here we describe a pulse sequence for efficiently creating singlets in the intermediate regime in a broad-band fashion. Singlet lifetimes are studied with a specially synthesized molecule over a wide range of magnetic fields using a home-built sample-lift apparatus. The experimental results are supplemented with spin simulations using parameters obtained from ab initio calculations. This work indicates that the chemical shift anisotropy (CSA) mechanism is relatively weak compared to singlet-triplet leakage for the proton system observed over a large magnetic field range. These experiments provide a mechanism for expanding the scope of singlet NMR to a larger class of molecules, and provide new insights into singlet lifetime limiting factors.
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