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Modern Physics Letters B

RYDBERG ELECTRON DYNAMICS IN EXTERNAL FIELDS

Jeroen Wals, Helen H. Fielding, H. B. van Linden van den Heuvell

Published Dec 30, 1995• 3 citations
Publisher

Abstract

We review the role which classical trajectories play in quantum-mechanical systems in a more or less chronological order guided by experimental observations. The onset of a renewed interest in classical dynamics was catalysed by the observation of unknown features in the absorption spectra of atoms in the presence of external magnetic and electric fields. Although the most dominant features in these spectra can be accounted for by the simple quantisation conditions for classical electrons, the finer details require a more sophisticated approach. Starting from the Feynman path-integral formalism, Gutzwiller’s periodic-orbit theory is introduced, which is then transformed into the closed-orbit theory developed by Delos et al. Applying this semiclassical theory enabled atomic physicists to understand complicated quantum spectra as a coherent sum of classical trajectories. Newly observed features such as core-scattered orbits and ghost orbits, necessitated adjustments to the standard closed-orbit theory in order to be able to reproduce these new features. Recent results from both scaled-energy experiments and wave-packet experiments are presented to demonstrate the classical dynamics underlying the quantum system as it is currently understood.

DOI
10.1142/s0217984995001844

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quant-pharXiv:2605.19019•May 20, 2026
We review the role which classical trajectories play in quantum-mechanical systems in a more or less chronological order guided by experimental observations. The onset of a renewed interest in classical dynamics was catalysed by the observation of unknown features in the absorption spectra of atoms in the presence of external magnetic and electric fields. Although the most dominant features in these spectra can be accounted for by the simple quantisation conditions for classical electrons, the finer details require a more sophisticated approach. Starting from the Feynman path-integral formalism, Gutzwiller’s periodic-orbit theory is introduced, which is then transformed into the closed-orbit theory developed by Delos et al. Applying this semiclassical theory enabled atomic physicists to understand complicated quantum spectra as a coherent sum of classical trajectories. Newly observed features such as core-scattered orbits and ghost orbits, necessitated adjustments to the standard closed-orbit theory in order to be able to reproduce these new features. Recent results from both scaled-energy experiments and wave-packet experiments are presented to demonstrate the classical dynamics underlying the quantum system as it is currently understood.
We analyze the spectra of simple Rydberg molecules in static fields within the framework of closed/periodic-orbit theories. We conclude that in addition to the usual classical orbits one must consider classically forbidden diffractive paths. Further, the molecule brings in a new type of "inelastic" diffractive trajectory in addition to the usual "elastic" diffractive orbits encountered in systems with point scatterers. The relative importance of inelastic versus elastic diffraction is quantified by merging the usual closed orbit theory framework with molecular quantum defect theory.
Diffraction and interference of matter waves are key phenomena in quantum mechanics. Here we present some results on particle diffraction in a wide variety of situations, ranging from simple slit experiments to more complicated cases such as atom scattering by corrugated metal surfaces and metal surfaces with simple and isolated adsorbates. The principal novelty of our study is the use of the so-called Bohmian formalism of quantum trajectories. These trajectories are able to satisfactorily reproduce the main features of the experimental results and, more importantly, they provide a causal intuitive interpretation of the underlying dynamics. In particular, we will focus our attention on: (a) a revision of the concepts of near and far field in undulatory optics; (b) the transition to the classical limit, where it is found that although the quantum and classical diffraction patterns tend to be quite similar, some quantum features are maintained even when the quantum potential goes to zero; and (c) a qualitative description of the scattering of atoms by metal surfaces in the presence of a single adsorbate.
In this chapter experiments on rubidium Rydberg atoms in external fields are reviewed [1 – 8]. In the first part results on the interaction of microwave radiation with rubidium Rydberg atoms are described. The Rydberg atoms interact with a microwave pulse of a well-defined duration. When applying coherent microwave radiation with a frequency exceeding a certain value, the experimentally observed microwave field strength at which 10% of the atoms are ionized has to be much larger than the value found by classical trajectory calculations. The atoms are stabilized by the dynamical localization. An extremely weak microwave broadband noise which is added to the coherent wave at least partially destroys the localization. This phenomenon depends on the bandwidth of the added noise. In further experiments the dependence of the 10% ionization microwave field strength on the duration τ of the microwave pulse has been investigated. For increasing noise level the 10% ionization field strength ∈ 0.1 develops from a behavior ∈ 0.1 ∼ τ −1/4 to a ∈ 0.1 ∼ τ −1/2 dependence, which is characteristic for a classical diffusion process. The second part of the chapter deals with experiments in strong static crossed electric and magnetic fields. Below as well as above the ionization energy the observed quasi-Landau(QL)-resonances are explained using classical trajectories. The ionization behavior of the QL-resonances is clearly influenced by the spatial structure of the associated classical orbits. In further experiments the dependence of the observed ionization energy on the magnetic field was investigated in the presence of a fixed static electric field.
This thesis is a theoretical study of the behavior of electrons in atoms and molecules subjected to external electromagnetic fields. Three electronic systems have been central in this work, the atomic and quasimolecular Rydberg states and the carbon allotrope graphene. The exaggerated properties of the highly excited Rydberg atoms, such as long lifetime, large spatial extension and low binding energy make them excellent candidates for both theoretical and experimental considerations. The analytical solutions of the hydrogen atom in quantum mechanics provide a good description for most Rydberg atoms. This is exploited in the work presented in this thesis and the accompanying papers, where we show results of numerical computations on interacting Rydberg atoms, with and without the presence of radiating fields, as well as dynamic Rydberg wave packets influenced by a train of femtosecond laser pulses. In the final part of the thesis the optical process of high-order harmonic generation in an extended molecular structure, represented by graphene, is considered. Rydberg atoms have a large dipole moment due to the large average electronic radius in the atom, which leads to a very strong dipole-dipole coupling between interacting particles in a gas of cold Rydberg atoms. This interaction, which is dependent on the internuclear separation between the atoms, induces a shift in the energy levels, which again prohibits the excitation of more than one atom in the gas, an effect commonly known as the Rydberg blockade. A correlated behavior is observed for the intrashell transitions in mutually excited Rydberg atoms. The microwave field driven dynamics is significantly supressed for internuclear distances below a given conditional radius which scales linearly with the principal quantum number n. Such an entangled electronic behavior may open for the realization of quantum gates applied in quantum informatics. The long-range interaction of Rydberg atoms is dominated by the dipole-dipole terms. Nevertheless, the investigation of two interacting Rydberg atoms, without the influence of electromagnetic radiation, has shown that the lower order multipolar terms play a vital role in the energy shifts as well as for the electronic probability distributions. We found that the energy curves, when including all multipole orders, correspond to both repulsive and attractive states with a stronger repulsion than attraction. We also propose a laser assisted approach for stabilization of Rydberg gases by controlled transitions between such attractive and repulsive energy states. Single-electron ionization of a dynamic Rydberg wave packet confined within a single energy level has been investigated. The ionization probability of an intrashell Rydberg wave packet depends strongly on the degree of polarization. For a wave packet driven repeatedly between the circular (least polarized) state and the linear (most polarized) state by a rotating microwave field and subjected to a train of femtosecond laser pulses, the ionization probability will depend crucially on the laser repetition rate and number of pulses. The angular-resolved ionization probability and energy distribution in the continuum are also influenced by these parameters. The last part of the thesis is devoted to the study of high-order harmonic generation (HHG) in graphene. In the simple man’s model HHG can be described by an electron that is ionized and driven in an external field, after which it returns to the parent atom and recombines, emitting a high-energy photon with frequency that is a multiple of the incident laser frequency. We show that the harmonic spectra obtained from the interaction with linearly as well as circularly polarized femtosecond lasers yield harmonics up the classical limit for extended molecules. In contrast to diatomic molecules, the stable grid structure of graphene ensures that the harmonic generation cutoff remains constant with increasing signal power as the graphene diameter extends beyond the classical limit. Additionally, for circularly polarized lasers harmonics exceeding the classical predictions have been observed.
Gutzwiller's trace formula has a central place in quantum chaos because it provides semiclassical approximations for quantum energy levels in classically chaotic systems by linking them to classical periodic orbits. In this didactic article, we discuss a derivation of the trace formula starting from the Feynman path integral. We then describe how the trace formula is used to explain universal features in the distribution of the quantum energy levels that are described by random matrix theory, and we give an overview of related work.