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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Exploration of the Laser-Assisted Clustering and Reactivity of Trimethylaluminum with and without NH_3
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Exploration of the Laser-Assisted Clustering and Reactivity of Trimethylaluminum with and without NH_3

机译：有和没有NH_3的三甲基铝的激光辅助团聚和反应性的探索

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This paper provides results concerning the clustering and laser-assisted reactivity in constrained pulsed gas expansions of trimethylaluminum (TMAl) with and without ammonia. In these experiments, TMAl is introduced with just an Ar buffer gas or co-expanded with ammonia into a high vacuum chamber through a dual-source pulsed nozzle assembly. Independent control of individual gas backing pressures is maintained, and the nozzle assembly can be cooled as well. The output of an ArF excimer laser (193 nm) is focused into the mixing and reaction region of the nozzle source, and a quadrupole mass spectrometer (QMS) is used to characterize the expansion products. Both pressure and laser power dependence studies are used to reveal the origins of individual mass spectral features. Under certain conditions, laser irradiation or expanding, neat TMAl results in the formation of (CH_3)_(4-x)H_(2-y)Al_2, where x = 0, 1 and y = 0, 1. During TMAl expansion with NH_3, the parent ion signal for the Lewis acid-base adduct (CH_3)_3Al: NH_3 is observed in the gas phase by the QMS. Laser photolysis of the TMAl/NH_3 gas mixture produces reactions involving both precursor and adduct molecules. Also, the formation of a new (CH_3)_3 AlNH_2 product as a result of NH_2 radical reactivity with the (CH_3)_3Al:NH_3 adduct, i.e., (CH_3)_3Al:NH_3 + NH_2 → (CH_3)_3 AlNH_2 = NH_3, is revealed. Diverse higher mass clusters with Al-N bonded nuclei, e.g., (CH_3)_kAl_l(NH_2)_m(NH)_n, have also been observed. Finally, a comparison of aluminum and gallium metal organic species reveals similar propensities for intermolecular association for the two metals.
机译：本文提供了有关在有和没有氨的情况下三甲基铝（TMAl）的受限制脉冲气体膨胀中的团聚和激光辅助反应性的结果。在这些实验中，TMAl仅通过Ar缓冲气体引入或通过双源脉冲喷嘴组件与氨共同膨胀进入高真空室。维持对各个气体背压的独立控制，并且喷嘴组件也可以冷却。 ArF准分子激光（193 nm）的输出聚焦到喷嘴源的混合和反应区域中，并且使用四极质谱仪（QMS）表征膨胀产物。压力和激光功率相关性研究均用于揭示各个质谱特征的起源。在某些条件下，激光辐照或膨胀，纯净的TMAl会形成（CH_3）_（4-x）H_（2-y）Al_2，其中x = 0，1和y = 0，1。 QMS在气相中观察到NH_3，即路易斯酸碱加合物（CH_3）_3Al：NH_3的母体离子信号。 TMAl / NH_3气体混合物的激光光解产生涉及前体和加合物分子的反应。同样，由于NH_2与（CH_3）_3Al：NH_3加合物的NH_2自由基反应性，即（CH_3）_3Al：NH_3 + NH_2→（CH_3）_3 AlNH_2 = NH_3，形成了新的（CH_3）_3 AlNH_2产物。揭示。还已经观察到具有Al-N键合核的各种更高质量的簇，例如（CH_3）_kAl_1（NH_2）_m（NH）_n。最后，对铝和镓金属有机物的比较显示出两种金属的分子间缔合的相似倾向。

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