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arXiv:nlin/0106014 · Physical Review Letters

Rydberg Molecules in External Fields: A Semiclassical Analysis

A. Matzkin, T. S. Monteiro

Published Sep 11, 2001• 25 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevlett.87.143002

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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.
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.
Abstract This PhD tutorial discusses ultra-long-range Rydberg molecules, the exotic bound states of a Rydberg atom and one or more ground state atoms immersed in the Rydberg electron’s wave function. This novel chemical bond is distinct from an ionic or covalent bond, and is accomplished by a very different mechanism: the Rydberg electron, elastically scattering off of the ground state atoms, exerts a weak attractive force sufficient to form the molecule in long-range oscillatory potential wells. In the last decade this topic has burgeoned into a vibrant and mature subfield of atomic and molecular physics following the rapidly developing capability of experiment to observe and manipulate these molecules. This tutorial focuses on three areas where this experimental progress has demanded more sophisticated theoretical descriptions: the structure of polyatomic molecules, the influence of electronic and nuclear spin, and the behavior of these molecules in external fields. The main results are a collection of potential energy curves and electronic wave functions which together describe the physics of Rydberg molecules. Additionally, to facilitate future progress in this field, this tutorial provides a general overview of the current state of experiment and theory.
For many purposes it is desirable to have an easily understandable and accurate picture of the atomic states. This is especially true for the highly excited states which exhibit features not present in the well known states hydrogen-like orbitals with usual values of the quantum numbers. It could be expected that such visualizations are readily available. Unfortunately, that is not the case. We illustrate the problems by showing several less fortunate earlier presentations in some scientifically most valuable works, and show more suitable visualizations for those cases. The selected cases are not chosen to criticize the authors' approach. Rather, we have taken these very important papers to underline the need for serious work with graphical representations which this work attempts to be a part of. In this text we discuss the problems encountered when visualizing Rydberg states, review some existing presentations and propose guidelines for applications. The focus of this work are so called Stark states and coherent elliptic states of Rydberg atoms. In the sections on elliptic states we show some quite novel geometric interpretations which should be very helpful in analysis of Rydberg state manipulations in external fields. Our demonstration examples involve only hydrogen-like states. However, the techniques and analysis are also relevant for Rydberg molecules and more complicated highly excited atomic and molecular systems.
It is shown that semiclassical path representations provide a well-suited framework for the description of the diffraction of Rydberg atoms by laser light. They allow one to relate the momentum exchange between the atomic center-of-mass motion and the laser field directly to elementary laser-assisted collisions between the excited Rydberg electron and the ionic core. Thus besides a convenient calculational tool they provide also direct physical insight into the underlying internal dynamics of the Rydberg atoms.
Periodic orbit (PO) theory can be used to make connections between the quantum energy eigenvalue spectrum and the closed orbits of the corresponding classical system. The two-dimensional annular billiard or circular disk system (namely, a particle in the plane confined between inner and outer infinite circular walls at fR≡Rin<Rout≡R where 0<f<1) is examined in the context of periodic orbit theory to illustrate several novel aspects of the PO analysis. Important features of this problem include (i) the appearance and disappearance of various features in the classical path length spectrum as a parameter (in this case f=Rin/Rout), is continuously varied, (ii) the presence of path length features which do not correspond to classical trajectories, but are rather due to purely wavelike phenomena (namely, diffraction around the inner annulus), and (iii) the study of the contribution of different regions in the energy eigenvalue space to different classes of classical trajectories. This last feature is a general observation about periodic orbit theory which can be usefully applied to a number of billiard systems. In addition, since the annular disk system is seldom studied in detail in either classical or quantum mechanics, we provide an appendix which reviews some of the more traditional connections between the classical and quantum probability densities for this geometry, exemplifying some of the important differences between one- and two-dimensional systems which arise from purely geometrical rather than kinematical effects.