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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Heteroleptic samarium(iii) halide complexes probed by fluorescence-detected L-3-edge X-ray absorption spectroscopy
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Heteroleptic samarium(iii) halide complexes probed by fluorescence-detected L-3-edge X-ray absorption spectroscopy

机译：通过荧光检测的L-3边缘X射线吸收光谱法探测的异虫钐（III）卤化物复合物

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摘要

The addition of various oxidants to the near-linear Sm(ii) complex [Sm(N-dagger dagger)(2)] (1), where N-dagger dagger is the bulky bis(triisopropylsilyl)amide ligand {N((SiPr3)-Pr-i)(2)}, afforded a family of heteroleptic three-coordinate Sm(iii) halide complexes, [Sm(N-dagger dagger)(2)(X)] (X = F, 2-F; Cl, 2-Cl; Br, 2-Br; I, 2-I). In addition, the trinuclear cluster [{Sm(N-dagger dagger)}(3)((2)-I)(3)((3)-I)(2)] (3), which formally contains one Sm(ii) and two Sm(iii) centres, was isolated during the synthesis of 2-I. Complexes 2-X are remarkably stable towards ligand redistribution, which is often a facile process for heteroleptic complexes of smaller monodentate ligands in lanthanide chemistry, including the related bis(trimethylsilyl)amide {N(SiMe3)(2)} (N). Complexes 2-X and 3 have been characterised by single crystal X-ray diffraction, elemental analysis, multinuclear NMR, FTIR and electronic spectroscopy. The L-1 fluorescence-detected X-ray absorption spectra recorded at the Sm L-3-edge for 2-X exhibited a resolved pre-edge peak defined as an envelope of quadrupole-allowed 2p 4f transitions. The X-ray absorption spectral features were successfully reproduced using time-dependent density functional theoretical (TD-DFT) calculations that synergistically support the experimental observations as well as the theoretical model upon which the electronic structure and bonding in these lanthanide complexes is derived.
机译：将各种氧化剂添加到近线性SM（II）复合物[SM（n-匕首匕首）（2）]（1）中，其中N-匕首匕首是庞大的双（三异丙基甲硅烷基）酰胺配体{n（（SIPR3 ）-PR-I）（2）}，得到了一种异常的三坐标SM（III）卤化物复合物，[SM（N-匕首匕首）（2）（2）（x）]（x = F，2-F; CL，2-CL; BR，2-BR; I，2-I）。此外，三核簇[{SM（n-匕首匕首）}（3）（（2）-I）（3）（（3）-I）（2）]（3），其正式含有一个SM（ II）和两个SM（III）中心在合成的2-I期间被隔离。复合物2-X对配体再分配显着稳定，这通常是镧系化学中较小单常型配体的异致络合物的容纳方法，包括相关双（三甲基甲硅烷基）酰胺{N（SIME3）（2）}（n）。复合物2-X和3的特征在于单晶X射线衍射，元素分析，多核NMR，FTIR和电子光谱。在2-X的SM L-3边缘记录的L-1荧光检测到的X射线吸收光谱表现出定义的预先边缘峰被定义为允许四极的2P 4F转变的封套。使用时间依赖性密度官能化理论（TD-DFT）计算成功再现了X射线吸收光谱特征，该计算协同支持实验性观察以及衍生在这些镧系元素中的电子结构和粘合的理论模型。

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