An efficient laser vaporization source for chemically modified metal clusters characterized by thermodynamics and kinetics
An efficient laser vaporization source for chemically modified metal clusters characterized by thermodynamics and kinetics
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DOI：
10.1063/1.5017588
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发表时间：
2018-02-01
影响因子：
1.6
通讯作者：
Heiz, Ulrich
中科院分区：
文献类型：
--
作者：
Masubuchi, Tsugunosuke;Eckhard, Jan F.;Heiz, Ulrich
提出了一种激光汽化簇源，该源具有用于簇聚集的空间和反应器体积，每个都配备有脉冲阀，用于高效气相生产化学改性金属簇。团簇源的性能通过 Ta 和 Ta 氧化物团簇阳离子 TaxOy+ (y >= 0) 的产生进行评估。结果表明，团簇源在较宽的质量范围内产生 TaxOy+，其金属氧比可以通过改变影响引入团簇源的反应物 O-2 量的脉冲持续时间来轻松控制。反应动力学模型表明，氧化物的生成发生在低于 300 K 的热化条件下，而金属簇核可能是在多余的热量下产生的。这些特征还有利于通过簇和簇源中的反应性分子之间的反应产生感兴趣的“反应中间体”，随后可以对其反应性测量进行质量选择。由 AIP 出版社出版。
A laser vaporization cluster source that has a room for cluster aggregation and a reactor volume, each equipped with a pulsed valve, is presented for the efficient gas-phase production of chemically modified metal clusters. The performance of the cluster source is evaluated through the production of Ta and Ta oxide cluster cations, TaxOy+ (y >= 0). It is demonstrated that the cluster source produces TaxOy+ over a wide mass range, the metal-to-oxygen ratio of which can easily be controlled by changing the pulse duration that influences the amount of reactant O-2 introduced into the cluster source. Reaction kinetic modeling shows that the generation of the oxides takes place under thermalized conditions at less than 300 K, whereas metal cluster cores are presumably created with excess heat. These characteristics are also advantageous to yield "reaction intermediates" of interest via reactions between clusters and reactive molecules in the cluster source, which may subsequently be mass selected for their reactivity measurements. Published by AIP Publishing.