论文标题

通过选择性超精细调整最大化动态核极化

Maximising Dynamic Nuclear Polarisation via Selective Hyperfine Tuning

论文作者

Hall, L. T., Broadway, D. A., Stacey, A., Simpson, D. A., Tetienne, J-P., Hollenberg, L. C. L.

论文摘要

动态核极化(DNP)是指通过将自旋极化从高度极化电子的集合转移到目标核分析物中来增加核磁共振测量中信号的一类技术。但是,这些技术需要应用强磁场来最大化电子自旋极化,从而限制了电子核(超细)自旋偶联和转移的途径。在这项工作中,我们表明,对于具有内在的零场分裂的电子自旋$ S \ geq1 $的系统,可以利用基于实验室框架交叉放松的单独的一类更强的超精美相互作用来提高DNP效率和产量,而在中度场上运行。我们在分析上检查了现有方法,并确定这种方法将极化转移到核合一集中的速率上最多可以比现有技术的数量级。在室温下,使用可光上极性的$ s = 1 $的氮气空位(NV)缺陷的电子自旋系统作为电子自旋极化的来源,在室温下实验证明了这一结果。最后,我们评估了这些基于NV的方法在NMR和MRI应用的钻石外部分子旋转宏观量的极化。

Dynamic nuclear polarisation (DNP) refers to a class of techniques used to increase the signal in nuclear magnetic resonance measurements by transferring spin polarisation from ensembles of highly polarised electrons to target nuclear analytes. These techniques, however, require the application of strong magnetic fields to maximise electron spin polarisation, limiting pathways for electron-nuclear (hyperfine) spin coupling and transfer. In this work we show that, for systems of electronic spin $S\geq1$ possessing an intrinsic zero-field splitting, a separate class of stronger hyperfine interactions based on lab-frame cross relaxation may be utilised to improve DNP efficiency and yield, whilst operating at moderate fields. We analytically review existing methods, and determine that this approach increases the rate of polarisation transfer to the nuclear ensemble by up to an order of magnitude over existing techniques. This result is demonstrated experimentally at room temperature using the optically polarisable $S=1$ electron spin system of the nitrogen vacancy (NV) defect in diamond as the source of electron spin polarisation. Finally we assess the utility of these NV-based approaches for the polarisation of macroscopic quantities of molecular spins external to the diamond for NMR and MRI applications.

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