论文标题
通过长寿命瞬态中间体转向超低反应
Steering ultracold reactions through long-lived transient intermediates
论文作者
论文摘要
控制反应的途径和结果是化学方面的广泛追求目标。在气相反应中,这通常是通过操纵反应物的特性(包括其翻译能,方向和内部量子态)来实现的。相反,在这里,我们通过其中间复合物影响反应的途径,通常太短暂而无法受到外部过程的影响。尤其是,钾 - 氨基钾(KRB)反应物的超速制备导致长期寿命的中间络合物(k $ _2 $ _2 $ rb $ _2^*$),这使我们能够将反应从其名义基地面途径中转移到其名义上的地面途径上,使用新的兴奋状态途径,使用1064 nm的激发源,使用了一个固有的固有型号,以固有量的固有型号,以固有一个固有的ultecte ultection solecte locection solect of Molection nm persect ofer sol。此外,通过监测激发光突然去除后复杂种群的变化,我们直接测量复合物的寿命为$ 360 \ pm 30 $ ns,这与基于Rice-Ramsperger-Kassel-Kassel-Kassel-Marcus(RRKM)统计理论的计算一致。我们的结果阐明了在超速分子实验中广泛观察到的两体损失的起源。此外,长的复合寿命与观察到的光启动途径结合起来,可以通过高分辨率探测复合物的结构,从而阐明了反应动力学。
Controlling the pathways and outcomes of reactions is a broadly pursued goal in chemistry. In gas phase reactions, this is typically achieved by manipulating the properties of the reactants, including their translational energy, orientation, and internal quantum state. In contrast, here we influence the pathway of a reaction via its intermediate complex, which is generally too short-lived to be affected by external processes. In particular, the ultracold preparation of potassium-rubidium (KRb) reactants leads to a long-lived intermediate complex (K$_2$Rb$_2^*$), which allows us to steer the reaction away from its nominal ground-state pathway onto a newly identified excited-state pathway using a laser source at 1064 nm, a wavelength commonly used to confine ultracold molecules. Furthermore, by monitoring the change in the complex population after the sudden removal of the excitation light, we directly measure the lifetime of the complex to be $360 \pm 30$ ns, in agreement with our calculations based on the Rice-Ramsperger-Kassel-Marcus (RRKM) statistical theory. Our results shed light on the origin of the two-body loss widely observed in ultracold molecule experiments. Additionally, the long complex lifetime, coupled with the observed photo-excitation pathway, opens up the possibility to spectroscopically probe the structure of the complex with high resolution, thus elucidating the reaction dynamics.