期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2020
卷号：117
期号：17
页码：9202-9207
DOI：10.1073/pnas.1917618117
出版社：The National Academy of Sciences of the United States of America
摘要：It has long been predicted that oscillatory behavior exists in reactivity as a function of collision energy for heavy–light–heavy (HLH) chemical reactions in which a light atom is transferred between two heavy atoms or groups of atoms, but direct observation of such a behavior in bimolecular reactions remains a challenge. Here we report a joint theoretical and crossed-molecular-beam study on the Cl CH 4 → HCl CH 3 reaction. A distinctive peak at a collision energy of 0.15 eV for the CH 3 ( v = 0) product was experimentally detected in the backward scattering direction. Detailed quantum-dynamics calculations on a highly accurate potential energy surface revealed that this feature originates from the reactivity oscillation in this HLH polyatomic reaction. We anticipate that such reactivity oscillations exist in many HLH reactions involving polyatomic reagents.
