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Journal of Physics B Atomic Molecular and Optical Physics

The shape of spectral lines of two-electron Rydberg atoms/ions: analytical solution

Eugene Oks

Published Mar 14, 2017• 4 citations
Publisher

Abstract

Abstract We consider an isolated two-electron Rydberg atom/ion, where the average distance of the inner electron from the nucleus is much smaller than the average distance of the outer Rydberg electron from the nucleus. We calculate analytically the shape of any spectral line emitted by the inner electron under the rotating electric field of the outer electron—by using the O 4 symmetry of hydrogenic atoms/ions. By applying the obtained analytical expressions to the example of the Ly-alpha line, we arrive, in particular, to a peculiar result . Namely, as the spectral line splits into several components, the most intense components exhibit a quadratic Stark effect with respect to the electric field of the outer electron (though it is linear with respect to the dipole moment of the inner electron), while one would intuitively expect a linear dependence on the electric field of the outer electron since the subsystem Z + e is hydrogenic. We provide a physical explanation of this peculiar result.

DOI
10.1088/1361-6455/aa66c4

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The shape of spectral lines of two-electron Rydberg atoms/ions: analytical solution

Eugene Oks

Institute of Physics eBooks•Nov 1, 2021•1 citation
Abstract We consider an isolated two-electron Rydberg atom/ion, where the average distance of the inner electron from the nucleus is much smaller than the average distance of the outer Rydberg electron from the nucleus. We calculate analytically the shape of any spectral line emitted by the inner electron under the rotating electric field of the outer electron—by using the O 4 symmetry of hydrogenic atoms/ions. By applying the obtained analytical expressions to the example of the Ly-alpha line, we arrive, in particular, to a peculiar result . Namely, as the spectral line splits into several components, the most intense components exhibit a quadratic Stark effect with respect to the electric field of the outer electron (though it is linear with respect to the dipole moment of the inner electron), while one would intuitively expect a linear dependence on the electric field of the outer electron since the subsystem Z + e is hydrogenic. We provide a physical explanation of this peculiar result.
The problem of Rydberg atomic spectra in crossed electric F and magnetic B fields (combined Stark–Zeeman effects), as well as an oscillating electric field are under consideration. The main problem is the great array of radiative transitions between the Rydberg atomic states. The different versions of semiclassical approaches are applied for the solution of the problem. New approximate selection rules are established to simplify the matrix elements of radiative transitions, making it possible to reduce the complex expressions of Gordon’s hypergeometric series to the trivial trigonometric functions. Simple analytical formulas for the dipole matrix elements of a Rydberg hydrogen-like atom in external crossed electric and magnetic fields for Hnα are obtained. The specific calculations are presented for n = 10 to 9 transition both for parallel and perpendicular orientations of F–B fields. The result of Blokhintsev for a single Stark component in oscillating field is generalized for the array of radiative transitions between Rydberg atomic states. Such spectra with large values of modulation index are compared with static ones.
Wave functions of a hydrogen atom perturbed by an electric field are calculated under the assumption of a first-order Stark effect. It is assumed that the strength of the perturbation field is constant and its direction rotates around a fixed axis with a constant angular velocity. The ground state of the atom is not affected by the perturbation field. The energy level of the first excited state of the perturbed atom splits into nine sub-levels. The Lymann alpha line emitted from the perturbed atom consists of seven components. In the case where the angular velocity of the field rotation is small, the structure of the line is similar to that of the line emitted from an atom perturbed by a static field. In the case where, the angular velocity is large, it is similar to that of the line emitted from an unperturbed atom.
Introduction Series of atomic spectral lines had been studied by emission from excited vapors even before Balmer described the regularity of the visible lines of hydrogen in 1884. However, direct excitation had been restricted to the few lowest-lying levels, particularly those accessible by electric dipole transitions from the ground state using classical light sources. The advent of tunable lasers in the 1970s changed such spectroscopic limitations enormonsly, allowing excitation to a very much larger number of states. Atoms in highly excited states, typically with principal quantum numbers n ≥ 10, are called Rydberg atoms. They are oversize, fragile states of significant intrinsic interest. They are very rare in nature because of their size and fragility, but they are found in interstellar space (H I regions). One of the best sources for comprehensive descriptions of Rydberg atoms and references to the literature describing their exploration is Ref. [120]. It describes their characteristic properties and behavior both classically and quantum mechanically, and especially their strongly enhanced interactions with external fields. The first thing to note is that Rydberg atoms are usually characterized by a single, highly excited electron while all the other electrons remain in their original states. Thus their properties are very nearly classical, and the atoms are much closer to the ideal hydrogen-like model of Chap. 7, along with appropriate quantum defects (see Chap. 10). The spectroscopy of such states is especially interesting because the active electron is much less perturbed by the other electrons in the atom than when it is in lower states. Moreover, there are some special circumstances in which the energy of a Rydberg state is degenerate with an atomic state having two electrons excited to lower levels, and such configurations yield further new information. Second, Rydberg atoms do not usually decay back to the ground state by emission of characteristic radiation, so their study is mediated by other techniques that reveal new and interesting properties. Such properties arise because Rydberg atoms have a huge dipole moment and very low binding energy resulting from the large average distance between the excited electron and the nucleus-plus-core of the rest of the atom with net charge e . Third, transitions between Rydberg states are quite different from those connecting to the ground state for at least three reasons.
The linear-Stark-effect approximation is employed to investigate the effects of electric fields on autoionizing doubly excited atomic states corresponding to relatively large values of the outer-electron principal quantum number nnn. By assuming that a statistical distribution of the inner-electron magnetic sublevels has been established, simple expressions are derived which relate the autoionization and radiative transition rates in the presence of an electric field to the respective field-free rates. It is pointed out that the multiphoton laser excitation of the doubly excited states can give rise to a nonstatistical distribution of the magnetic sublevels and to complex interference terms involving transition amplitudes associated with different values of the outer-electron angular momentum quantum number lll. The results of calculations are presented for the autoionization and radiative-transition rates which play the most important role in the dielectronic recombination of the Li-like Fe+23{\mathrm{Fe}}^{+23}Fe+23 ion through the $2p\ensuremath{\rightarrow}2s$ inner-electron transition, where the contributions from large-nnn values are particularly important. In these calculations it is assumed that the magnetic sublevels are statistically populated and only the simple expressions for the transition rates are employed. The effects of the electric field on the dominant (inner-electron) radiative decay rate can be neglected, but the electric field mixing of the outer-electron lll substates substantially increases the autoionization rates from the higher-lll sublevels.
The theory of collisions of Rydberg atoms with rare-gas atoms is generalized to include the effects of an applied static electric field. Two effects occur. First, the field causes the states to split, and the increased energy separations lead to a decrease in the inelastic cross sections. Second, there is a change in the form of the wave functions, because the various Stark states in the field have electron charge distributions that may be localized in very different regions of space. The present work focuses on this second effect. With the description of the initial and final Stark states of the Rydberg atom by the proper electronic wave functions obtained in parabolic coordinates, cross sections are obtained for a variety of specific transitions of Rydberg atoms (n=10,15,and20n=10, 15, \mathrm{and} 20n=10,15,and20) caused by collisions. The calculations are strictly valid for hydrogen, but exhibit general features that are expected to apply to other Rydberg atoms as well. The results show a dramatic effect on the cross section for particular transitions depending on the degree of overlap of the initial and final charge distributions. In addition, it is observed that transitions are favored that involve small changes in the azimuthal quantum number mmm. The origin of this tendency is discussed.