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通过扫频-parahydrogen 诱导的 C 极化的恒绝热磁场扫描来探测核自旋能级交叉。

Scanning Nuclear Spin Level Anticrossings by Constant-Adiabaticity Magnetic Field Sweeping of Parahydrogen-Induced C Polarization.

机构信息

Department of Chemistry, Integrative Biosciences (IBio), Karmanos Cancer Institute (KCI), Wayne State University, Detroit, Michigan 48202, United States.

Russian Academy of Sciences, Leninskiy Prospekt 14, Moscow 119991, Russia.

出版信息

J Phys Chem Lett. 2022 Mar 3;13(8):1925-1930. doi: 10.1021/acs.jpclett.2c00029. Epub 2022 Feb 18.

Abstract

The polarization transfer between H protons and C heteronuclei is of central importance in the development of parahydrogen-based hyperpolarization techniques dedicated to the production of C-hyperpolarized molecular probes. Here we unveil the spin conversion efficiency in the polarization transfer between parahydrogen-derived protons and C nuclei of an ethyl acetate biomolecule, formed by the homogeneous hydrogenation of vinyl acetate with parahydrogen, obtained by applying constant-adiabaticity sweep profiles at ultralow magnetic fields. The experiments employed natural C-13 abundance. Spin level anticrossings can be detected experimentally using a scanning approach and are selected to improve the polarization transfer efficiency. C polarization of up to 12% is readily achieved on the carbonyl center. The results demonstrate the simplicity, reproducibility, and high conversion efficiency of the technique, opening the door for a refined manipulation of hyperpolarized spins in both basic science experiments (., state-selected spectroscopy in the strong-coupling regime) and biomedical nuclear magnetic resonance applications.

摘要

在开发用于生产 C 超极化分子探针的基于 Para 氢气的超极化技术中,H 质子和 C 杂核之间的极化转移至关重要。在这里,我们揭示了通过应用超低频磁场中的恒绝热性扫频曲线,由醋酸乙烯酯与 Para 氢气均匀氢化形成的醋酸乙酯生物分子中,Para 氢气衍生的质子与 C 核之间的自旋转换效率。实验采用了自然丰度的 C-13。自旋能级交叉可以通过扫描方法进行实验检测,并被选择用于提高极化转移效率。在羰基中心上很容易达到高达 12%的 C 极化。结果证明了该技术的简单性、可重复性和高转换效率,为在基础科学实验(例如,强耦合态下的态选择性光谱学)和生物医学磁共振应用中对超极化自旋进行精细操作开辟了道路。

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