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Atoms

Redistribution of the Rydberg State Population Induced by Continuous-Spectrum Radiation

Anastasia S. Chervinskaya, Dmitrii L. Dorofeev, B. A. Zon

Published Aug 6, 2021• 2 citations
Publisher

Abstract

We consider the redistribution of the Rydberg state population resulting from multistep cascade transitions induced by radiation with a continuous spectrum. The population distribution is analyzed within the space of quantum numbers n and l. The dynamics of the system are studied using both the numerical solution of kinetic equations and the diffusion approximation based on the Fokker–Planck equation. The main path of the redistribution process is determined.

DOI
10.3390/atoms9030055

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arXiv:2012.11485•Nature Communications•Jun 23, 2021•16 citations
We consider the redistribution of the Rydberg state population resulting from multistep cascade transitions induced by radiation with a continuous spectrum. The population distribution is analyzed within the space of quantum numbers n and l. The dynamics of the system are studied using both the numerical solution of kinetic equations and the diffusion approximation based on the Fokker–Planck equation. The main path of the redistribution process is determined.
Abstract Redistribution of population of Rydberg states and ionization of an atom as a result of multistep cascade transitions between states induced by radiation with continuous spectrum are analyzed. Analysis is carried out both by straightforward numerical solution of kinetic equations governing state populations and by using the diffusion approximation based on the Fokker–Planck equation. Using an example of a sodium atom exposed to radiation with rectangular spectrum as an example, we demonstrate good agreement between the diffusion approximation and numerical solution to kinetic equations. Estimates for state populations, ionization rate, and minimum spectral density of radiation required for achieving considerable ionization are obtained within the framework of the diffusion approximation.
Redistribution of population and ionization of atomic Rydberg states due to multistep cascade transitions between states under the influence of radiation with continuous spectrum is considered. Consideration is carried up both by simulation of kinetic equations for state populations and with the use of a diffusion approximation based on the Fokker-Planck equation. On the example of sodium atom under the influence of radiation with rectangular spectrum a good agreement between the diffusion approximation and the kinetic equation simulation is shown. In the frame of the diffusion approximation some estimations are derived for the state populations, ionization rates and minimal spectral density of radiation necessary for significant ionization.
Our recent approximate analytical results on the evolution of the initial state and the excitation from this state of a band of high Rydberg states by an optical pulse [Phys. Rev. A 55, 2144 (1997)] are compared with more exact numerical results. The difference between the two approaches is that the approximations of representative atom-field couplings and equidistant spacing of high Rydberg states, applied in the analytical model, are removed in the numerical model. We find that the approximate analytical model is not able to reproduce all the results of the more exact numerical model, if the laser pulse is very short (i.e., much shorter that the Kepler period of the resonantly excited high Rydberg state) or very intense (i.e., when the Rabi period for the resonant transition is substantially shorter than the above Kepler period). This mainly concerns the redistribution of the population over different Rydberg states. The analytical model predicts a symmetric distribution centered around the resonantly excited Rydberg state, irrespective of the pulse duration and intensity, while the numerical model allows an asymmetric distribution with its maximum shifted towards lower Rydberg states. Despite the above-stated difference, the analytical model is able to give preliminary results for the total population of all the excited Rydberg states and the evolution of the initial state, imitating at least qualitatively the results of the numerical model in certain time and intensity scales.
A stochastic model of associative ionization in collisions of Rydberg atoms with ground-state atoms is presented. The conventional Duman–Shmatov–Mihajlov–Janev (DSMJ) model treats the ionization as excitation of Rydberg electron to the continuum by the electric-dipole field generated by exchange interaction within the quasi-molecular ion. The stochastic model essentially extends this treatment by taking into account redistribution of population over a range of Rydberg states prior to ionization, which is caused by non-adiabatic processes in overlapping multiple level crossings of quasi-molecular Rydberg states. The redistribution is modelled as diffusion of electrons in the Rydberg energy spectrum using a Fokker–Planck-type equation. The process of l -mixing of Rydberg states at large internuclear distances and twisting of the collision trajectories on attractive potentials are taken into account. The choice of the collision velocity distribution is also shown to be important. Associative ionization rates have been calculated for Na**( nl ) + Na collisions with n = 5–25 and l = 0, 1, 2, and compared with the available experimental data and the calculations performed using the nonlinear DSMJ model. At relatively low n the stochastic model yields a substantially better agreement with the experimental data than the DSMJ model, while the results of both models converge at large n .
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.
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.