Okada Kunihiro, Sakimoto Kazuhiro, Takada Yusuke, Schuessler Hans A
Department of Physics, Sophia University, 7-1 Kioicho, Chiyoda, Tokyo 102-8554, Japan.
Department of Physics and Astronomy, Texas A&M University, College Station, Texas 77843-4242, USA.
J Chem Phys. 2020 Sep 28;153(12):124305. doi: 10.1063/5.0013807.
We have measured the translational temperature dependence of the reaction rate constant for CHCN + Ne → products at low temperatures. A cold Ne ensemble was embedded in Ca Coulomb crystals by a sympathetic laser cooling technique, while cold acetonitrile (CHCN) molecules were produced by two types of Stark velocity filters to widely change the translational temperatures. The measured reaction rate constant gradually increases with the decrease in the translational temperature of the velocity-selected CHCN molecules from 60 K down to 2 K, and thereby, a steep increase was observed at temperatures lower than 5 K. A comparison between experimental rate constants and the ion-dipole capture rate constants by the Perturbed Rotational State (PRS) theory was performed. The PRS capture rate constant reproduces well the reaction rate constant at a few kelvin but not for temperatures higher than 5 K. The result indicates that the reaction probability is small compared to typical ion-polar molecule reactions at temperatures above 5 K.
我们测量了低温下CHCN + Ne → 产物反应速率常数的平动温度依赖性。通过交感激光冷却技术将冷的氖原子团嵌入钙库仑晶体中,同时通过两种类型的斯塔克速度过滤器产生冷的乙腈(CHCN)分子,以广泛改变平动温度。所测量的反应速率常数随着速度选择的CHCN分子的平动温度从60 K降低到2 K而逐渐增加,因此,在低于5 K的温度下观察到急剧增加。通过微扰转动态(PRS)理论对实验速率常数和离子 - 偶极捕获速率常数进行了比较。PRS捕获速率常数在几开尔文时能很好地再现反应速率常数,但在高于5 K的温度下则不然。结果表明,在高于5 K的温度下,与典型的离子 - 极性分子反应相比,该反应的概率较小。