Understanding the Effect of an Amorphous Surface on the Ultrafast Dynamics of a Heterogeneous Photoinduced Reaction: CD 3 I Photoinduced Reaction on Amorphous Cerium Oxide Films
Understanding the Effect of an Amorphous Surface on the Ultrafast Dynamics of a Heterogeneous Photoinduced Reaction: CD 3 I Photoinduced Reaction on Amorphous Cerium Oxide Films
复制标题
了解非晶表面对异质光诱导反应超快动力学的影响：非晶氧化铈薄膜上的 CD 3 I 光诱导反应
DOI：
10.1021/acs.jpclett.2c02294
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Vaida, Mihai E.
中科院分区：
文献类型：
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作者：
Pathan, Md Afjal;Gupta, Aakash;Vaida, Mihai E.
在这项工作中，要了解如何无定形表面影响表面光致反应的动力学，泵探测光谱结合质谱跟踪超快演化的中间体和最终产品的时间，质量和能量分辨率。作为模型体系，研究了CD_3I吸附在非晶氧化铈薄膜上的光诱导反应。在新制备的表面上产生的第一中间体的一部分被捕获以使表面钝化。在A带激发后，CD3I的最小解离时间表明，CD3I吸附几何与CD3或I面对气相存在，然而，瞬态数据表明，大多数分子吸附与I原子面对表面。CD 3和I被消耗形成I 2和改革CD 3 I，只有在中间体失去了光解释放的过量平移能后，它们才以稳定的速率产生。
In this work, to understand how an amorphous surface influences the dynamics of surface photoinduced reactions, pump–probe spectroscopy in conjunction with mass spectrometry is employed to track the ultrafast evolution of intermediates and final products with time, mass, and energy resolution. As a model system, the photoinduced reaction of CD3I adsorbed on amorphous cerium oxide films is investigated. A fraction of the first intermediates produced on a freshly prepared surface is trapped to passivate the surface. After the A-band excitation, the minimum dissociation time of CD3I indicates that CD3I adsorption geometries with either CD3or I facing the gas phase exist; however, the transient data suggest that most molecules are adsorbed with the I atom facing the surface. CD3and I are consumed to form I2and reform CD3I, which are produced at a steady rate only after the intermediates have lost the excess translational energy released from photodissociation.