Extending 17O transverse relaxation measurement to satellite transitions as a direct probe of molecular dynamics in solids

IF 1.8 3区化学 Q4 CHEMISTRY, PHYSICAL

Solid state nuclear magnetic resonance Pub Date : 2025-04-15 DOI:10.1016/j.ssnmr.2025.102004

Yizhe Dai , Ivan Hung , Zhehong Gan , Gang Wu

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引用次数: 0

Abstract

We report utilization of transverse relaxation rate (R₂) of ¹⁷O (I = 5/2) satellite transitions (STs) as a probe of molecular dynamics in solids. A simple theoretical model using spectral density functions is proposed to describe the general R₂ behaviors of half-integer quadrupolar nuclei in solids in the presence of molecular motion (or chemical exchange). Experimental ¹⁷O R₂ data recorded for both CT and ST from ¹⁷O-labeled NaNO₂ over a large temperature range are used to verify the theoretical predictions. Our theoretical model is shown to be fully consistent with a full quantum mechanical treatment of the chemical exchange problem involving half-integer quadrupolar nuclei in solids by numerically solving the Liouville-von Neumann equation. The new ¹⁷O ST R₂ method was also applied to study the carboxylate flipping motion in two [¹⁷O]carboxylic acid-pyridine adducts in the solid state. The advantages of the ST R₂ approach are discussed. This ST R₂ approach adds a new dimension to the currently available CT-based solid-state NMR techniques for probing molecular motion in solids.

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将 17O 横向弛豫测量扩展到卫星跃迁，作为固体分子动力学的直接探针

我们报道了利用17O （I = 5/2）卫星跃迁（STs）的横向弛豫率（R2）作为固体分子动力学的探针。提出了一种简单的理论模型，利用谱密度函数来描述固体中存在分子运动（或化学交换）的半整数四极核的一般R2行为。实验用17O标记的NaNO2在大温度范围内记录的CT和ST的17O R2数据用于验证理论预测。通过数值求解Liouville-von Neumann方程，我们的理论模型与固体中涉及半整数四极核的化学交换问题的全量子力学处理完全一致。采用新的17O ST R2方法研究了两种[17O]羧酸-吡啶加合物在固体状态下的羧酸翻转运动。讨论了str2方法的优点。这种str2方法为目前可用的基于ct的固态核磁共振技术增加了一个新的维度，用于探测固体中的分子运动。

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来源期刊

Solid state nuclear magnetic resonance 物理-光谱学

CiteScore

5.30

自引率

9.40%

发文量

审稿时长

72 days

期刊介绍： The journal Solid State Nuclear Magnetic Resonance publishes original manuscripts of high scientific quality dealing with all experimental and theoretical aspects of solid state NMR. This includes advances in instrumentation, development of new experimental techniques and methodology, new theoretical insights, new data processing and simulation methods, and original applications of established or novel methods to scientific problems.