Geppert Philipp, Althön Max, Fichtner Daniel, Ott Herwig
Department of Physics and Research Center OPTIMAS, Technische Universität Kaiserslautern, Kaiserslautern, Germany.
Nat Commun. 2021 Jun 23;12(1):3900. doi: 10.1038/s41467-021-24146-0.
Exploring the dynamics of inelastic and reactive collisions on the quantum level is a fundamental goal in quantum chemistry. Such collisions are of particular importance in connection with Rydberg atoms in dense environments since they may considerably influence both the lifetime and the quantum state of the scattered Rydberg atoms. Here, we report on the study of state-changing collisions between Rydberg atoms and ground state atoms. We employ high-resolution momentum spectroscopy to identify the final states. In contrast to previous studies, we find that the outcome of such collisions is not limited to a single hydrogenic manifold. We observe a redistribution of population over a wide range of final states. We also find that even the decay to states with the same angular momentum quantum number as the initial state, but different principal quantum number is possible. We model the underlying physical process in the framework of a short-lived Rydberg quasi-molecular complex, where a charge exchange process gives rise to an oscillating electric field that causes transitions within the Rydberg manifold. The distribution of final states shows a diffusive-like behavior.
在量子水平上探索非弹性碰撞和反应性碰撞的动力学是量子化学的一个基本目标。此类碰撞在与密集环境中的里德堡原子相关的研究中尤为重要,因为它们可能会对散射的里德堡原子的寿命和量子态产生相当大的影响。在此,我们报告了关于里德堡原子与基态原子之间状态变化碰撞的研究。我们采用高分辨率动量光谱法来确定最终状态。与之前的研究不同,我们发现此类碰撞的结果并不局限于单一的类氢多重态。我们观察到在广泛的最终状态范围内存在布居的重新分布。我们还发现,即使是衰变到与初始状态具有相同角动量量子数但主量子数不同的状态也是可能的。我们在一个短寿命的里德堡准分子复合体框架内对潜在的物理过程进行建模,其中电荷交换过程会产生一个振荡电场,该电场会导致里德堡多重态内的跃迁。最终状态的分布呈现出类似扩散的行为。