Chadwick Helen, Beck Rainer D
Laboratoire de Chimie Physique Moléculaire, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland; email:
Annu Rev Phys Chem. 2017 May 5;68:39-61. doi: 10.1146/annurev-physchem-052516-044910. Epub 2017 Jan 11.
Chemical reactions at the gas-surface interface are ubiquitous in the chemical industry as well as in nature. Investigating these processes at a microscopic, quantum state-resolved level helps develop a predictive understanding of this important class of reactions. In this review, we present an overview of the field of quantum state-resolved gas-surface reactivity measurements that explore the role of the initial quantum state on the dissociative chemisorption of a gas-phase reactant incident on a solid surface. Using molecular beams and either quantum state-specific reactant preparation or product detection by laser excitation, these studies have observed mode specificity and bond selectivity as well as steric effects in chemisorption reactions, highlighting the nonstatistical and complex nature of gas-surface reaction dynamics.
气-固表面界面处的化学反应在化学工业以及自然界中普遍存在。在微观、量子态分辨水平上研究这些过程有助于对这类重要反应形成预测性的理解。在本综述中,我们概述了量子态分辨气-固表面反应性测量领域,该领域探讨了初始量子态对气相反应物入射到固体表面时的解离化学吸附的作用。通过分子束以及量子态特异性反应物制备或激光激发产物检测,这些研究观察到了化学吸附反应中的模式特异性、键选择性以及空间效应,突出了气-固表面反应动力学的非统计性和复杂性。