通过受控激发至极端转动态增强 SiO$^+$ 离子的反应活性
Enhancing reactivity of SiO$^+$ ions by controlled excitation to extreme rotational states
AI总结：
本研究在离子阱中利用宽带光泵浦将 SiO$^+$ 制备至 j 高达170的超转子态，发现极端转动激发可显著增强其与 H$_2$ 的夺氢反应速率，并通过理论揭示过渡态处转动模式与反应坐标的强耦合机制。
摘要：
分子的光泵浦为在广泛转动能量范围内控制化学反应提供了独特机会。本工作报告了一种反应物受到极端转动激发的化学反应，并对其进行了动力学表征。我们在离子阱中研究了夺氢反应 SiO$^+$ + H$_2$ → SiOH$^+$ + H 的化学反应活性。采用宽带光泵浦方法，将 SiO$^+$ 阳离子制备在狭窄的转动态分布中，其中包括转动量子数 $\it{(j)}$ 高达170的超转子态。我们表明，SiO$^+$ 的超转子态显著提高了反应速率，这一趋势也由互补的理论研究所复现。我们揭示，反应活性转动增强的机制是：在主导动力学路径上，SiO$^+$ 转动模式与过渡态处的反应坐标之间存在强耦合。
英文摘要：
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.
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