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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Pulsed ENDOR Study of Water Coordination to Gd~(3+) Complexes in Orientationally Disordered Systems
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Pulsed ENDOR Study of Water Coordination to Gd~(3+) Complexes in Orientationally Disordered Systems

机译：定向失序系统中水与Gd〜（3+）配合物的脉冲ENDOR研究

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In orientationally disordered systems, the ENDOR (electron-nuclear double resonance) spectra of high-spin ions having weak crystal field interaction (cfi) contain nuclear transition lines (often overlapped) that belong to several different electron spin manifolds, and the transition lines for each manifold are distorted by the effect of the cfi. In this work, we have shown that, although the latter distortions can be quite considerable in a general case, the statistical distributions of the cfi parameters and orientations of the cfi axes in glassy samples result in ENDOR line shapes similar to the usual powder pattern determined by the hyperfine interaction only, which greatly simplifies their analysis. We have also shown that the two-dimensional Mims ENDOR technique can be used to disentangle the nuclear transitions that belong to different electron spin manifolds. The results of the analysis were applied to study the Gd~(3+) aquo complex and the Gd~(3+)-based MRI contrast agent GdHPDO3A in frozen glassy water/methanol solutions. The average distance between Gd and protons of the water ligands was found to be about 3.1 A for both complexes.
机译：在取向混乱的系统中，具有弱晶体场相互作用（cfi）的高自旋离子的ENDOR（电子-核双共振）光谱包含属于几个不同电子自旋流形的核跃迁线（通常是重叠的），以及每个歧管由于cfi的作用而变形。在这项工作中，我们已经表明，尽管在一般情况下后者的畸变可能相当大，但是玻璃样品中cfi参数的统计分布和cfi轴方向的分布导致ENDOR线形类似于确定的通常粉末图案仅通过超精细相互作用，就大大简化了它们的分析。我们还表明，二维Mims ENDOR技术可用于解开属于不同电子自旋流形的核跃迁。分析结果用于研究在冷冻玻璃水/甲醇溶液中基于Gd〜（3+）的水性复合物和基于Gd〜（3+）的MRI造影剂GdHPDO3A。发现两种配合物的Gd与水配体的质子之间的平均距离约为3.1A。

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