Quantum state-resolved gas/surface reaction dynamics probed by reflection absorption infrared spectroscopy
Quantum state-resolved gas/surface reaction dynamics probed by reflection absorption infrared spectroscopy
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DOI：
10.1063/1.4803933
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发表时间：
2013-05-01
影响因子：
1.6
通讯作者：
Beck, Rainer D.
中科院分区：
文献类型：
--
作者：
Chen, Li;Ueta, Hirokazu;Beck, Rainer D.
报道了一种新的分子束/表面科学装置的设计和表征，该装置用于气体/表面反应动力学的量子态分辨研究，将通过快速绝热通道在分子束中制备光学状态特定的反应物与通过反射吸收红外光谱(RAIRS)检测表面结合的反应产物相结合。RAIRS是一种非侵入性红外光谱检测技术，能够在线监测分子束在反应物沉积过程中反应产物在目标表面的堆积情况。通过校准的RAIRS检测获得的产物摄取速率得到了依赖于覆盖率的状态分辨反应概率S(θ)。此外，RAIRS技术获得的吸附产物的红外吸收光谱提供了结构信息，有助于识别新生的反应产物，研究反应途径，并确定化学吸附反应不同途径的支化比。用这个新装置测量了甲烷在铂(111)上的解离化学吸附，以说明RAIRS探测对于非常详细地研究气体/表面界面上的化学反应是有用的。(C)2013 AIP出版有限责任公司。
We report the design and characterization of a new molecular-beam/surface-science apparatus for quantum state-resolved studies of gas/surface reaction dynamics combining optical state-specific reactant preparation in a molecular beam by rapid adiabatic passage with detection of surface-bound reaction products by reflection absorption infrared spectroscopy (RAIRS). RAIRS is a non-invasive infrared spectroscopic detection technique that enables online monitoring of the buildup of reaction products on the target surface during reactant deposition by a molecular beam. The product uptake rate obtained by calibrated RAIRS detection yields the coverage dependent state-resolved reaction probability S(theta). Furthermore, the infrared absorption spectra of the adsorbed products obtained by the RAIRS technique provide structural information, which help to identify nascent reaction products, investigate reaction pathways, and determine branching ratios for different pathways of a chemisorption reaction. Measurements of the dissociative chemisorption of methane on Pt(111) with this new apparatus are presented to illustrate the utility of RAIRS detection for highly detailed studies of chemical reactions at the gas/surface interface. (C) 2013 AIP Publishing LLC.