Lindale Jacob R, Warren Warren S
Department of Chemistry, Duke University, Durham, NC 27708, USA.
Departments of Physics, Biomedical Engineering, and Radiology, Duke University, Durham, NC 27708, USA.
Sci Adv. 2025 Feb 21;11(8):eadq9974. doi: 10.1126/sciadv.adq9974. Epub 2025 Feb 19.
Coherent evolution is punctuated by dynamical processes such as chemical exchange, conformational transformation, or site hopping in many important problems ranging from biomolecular function to ion trap quantum computation. One well-explored example is nuclear magnetic resonance (NMR) spectroscopy, where experimental development is grounded in decades-old theory, but structural dynamics are not easily integrated into this picture. Here, we introduce an approach that selectively excites NMR resonances that undergo chemical exchange while suppressing the signal arising from nondynamic components of the system. We show that for exchange rates spanning more than four orders of magnitude, one can still selectively excite spins undergoing exchange while suppressing static resonances. Generalizing this approach, to selectively excite (or selectively preserve) only members of an ensemble that have undergone exchange or rearrangement, has the potential to improve the analytical power of many spectroscopic techniques.
在从生物分子功能到离子阱量子计算等许多重要问题中,相干演化会被诸如化学交换、构象转变或位点跳跃等动力学过程所打断。一个得到充分研究的例子是核磁共振(NMR)光谱学,其实验发展基于数十年前的理论,但结构动力学却不易融入这幅图景。在这里,我们介绍一种方法,该方法能选择性地激发经历化学交换的NMR共振,同时抑制系统中非动态成分产生的信号。我们表明,对于跨越四个以上数量级的交换速率,人们仍然可以在抑制静态共振的同时选择性地激发经历交换的自旋。推广这种方法,即仅选择性地激发(或选择性地保留)集合中经历过交换或重排的成员,有可能提高许多光谱技术的分析能力。