论文标题
通过对极端旋转状态的受控激发来增强SIO $^+$离子的反应性
Enhancing reactivity of SiO$^+$ ions by controlled excitation to extreme rotational states
论文作者
论文摘要
分子的光学泵送为控制各种旋转能的化学反应提供了独特的机会。这项工作报告了反应物的极端旋转激发及其动力学表征的化学反应。我们调查了氢抽象反应的化学反应性Sio $^ + $ + H $ _2 $ $ \ rightarrow $ sioh $^ + $ + $ + h in Ion陷阱中。 SIO $^+$ cation是在狭窄的旋转状态分布中制备的,包括使用宽带光学泵送方法的旋转量子数$ \ it {(j)} $的超级旋转状态。我们表明,SIO $^+$的超级转子状态显着提高了反应率,这是通过互补理论研究复制的趋势。我们揭示了反应性旋转增强的机制,是SIO $^+$旋转模式与反应坐标在主要动力学途径上的过渡状态的强耦合。
Optical pumping of molecules provides unique opportunities for control of chemical reactions at a wide range of rotational energies. This work reports a chemical reaction with extreme rotational excitation of a reactant and its kinetic characterization. We investigate the chemical reactivity for the hydrogen abstraction reaction SiO$^+$ + H$_2$ $\rightarrow$ SiOH$^+$ + H in an ion trap. The SiO$^+$ cations are prepared in a narrow rotational state distribution, including super-rotor states with rotational quantum number $\it{(j)}$ as high as 170, using a broad-band optical pumping method. We show that the super-rotor states of SiO$^+$ substantially enhance the reaction rate, a trend reproduced by complementary theoretical studies. We reveal the mechanism for the rotational enhancement of the reactivity to be a strong coupling of the SiO$^+$ rotational mode with the reaction coordinate at the transition state on the dominant dynamical pathway.