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Abstract
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.
Highlights
Exploring the dynamics of inelastic and reactive collisions on the quantum level is a fundamental goal in quantum chemistry
Today, such processes are important for low-temperature plasma physics[2], astrophysical plasmas[3], and ultracold atom experiments, which have found in Rydberg physics a perfect match to explore ultracold chemistry and many-body physics: On the one hand, the high control over the internal and external degrees of freedom in an ultracold atomic gas enables the study of new phenomena in the field of Rydberg physics, such as Rydberg molecules[4], Rydberg blockade[5], Rydberg antiblockade[6,7], and coherent many-body dynamics[8]
The microscopic details of such a collision involve the physics of ULRMs4, where s- and p-wave scattering between the Rydberg electron and the ground state atom determine the potential energy landscape at large internuclear distances
Summary
Exploring the dynamics of inelastic and reactive collisions on the quantum level is a fundamental goal in quantum chemistry. The same control can be used to study established processes in a detailed fashion, unraveling the underlying microscopic physical mechanisms This way, the stateresolved study of inelastic collisions and molecular decay processes involving Rydberg atoms has become possible. The microscopic details of such a collision involve the physics of ULRMs4, where s- and p-wave scattering between the Rydberg electron and the ground state atom determine the potential energy landscape at large internuclear distances. Inspired by the MOTRIMS technique, we have developed a high-resolution momentum microscope, which enables the study of inelastic processes involving Rydberg atoms
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