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Physical Review A

Stark structure of the Rydberg states of alkali-metal atoms

Myron L. Zimmerman, Michael G. Littman, Michael M. Kash, Daniel Kleppner

Published Dec 1, 1979• 658 citations
Publisher

Abstract

The authors describe practical methods for calculating the Stark structure of Rydberg states of the alkali metals based on diagnolization of the energy matrix. A survey of Stark structures is presented for all of the alkali metals in the vicinity of $n=15$. Topics discussed include general methods for evaluating radial matrix elements, the treatment of fine structure, oscillator-strength distribution, scaling laws, the structure of a level anticrossing, and sources of error. Experimental Stark maps are compared with calculated results for lithium and cesium. Experimental studies of the oscillator-strength distribution within a Stark manifold and the structure of a level anticrossing are also presented.

DOI
10.1103/physreva.20.2251

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Physical Review Letters•Apr 5, 1976•112 citations
The authors describe practical methods for calculating the Stark structure of Rydberg states of the alkali metals based on diagnolization of the energy matrix. A survey of Stark structures is presented for all of the alkali metals in the vicinity of n=15n=15n=15. Topics discussed include general methods for evaluating radial matrix elements, the treatment of fine structure, oscillator-strength distribution, scaling laws, the structure of a level anticrossing, and sources of error. Experimental Stark maps are compared with calculated results for lithium and cesium. Experimental studies of the oscillator-strength distribution within a Stark manifold and the structure of a level anticrossing are also presented.
The Stark effects of the Rydberg states in the alkaline-earth atoms are studied theoretically. Using a method similar to the treatment of alkali atoms, the properties of the Stark states of Mg, Ca, Sr and Ba atoms in the regions far away from the perturbers are investigated. The Stark maps for Mg ( n = 16, M = 0), Ca ( n = 10, M = 0), Sr ( n = 12, M = 0) and Ba ( n = 13, | M | = 0, 1) are presented. Topics such as the general methods of calculation, the treatment of fine structure and the structure of level anti-crossings are discussed. The comparison between the theoretical and experimental Stark maps is satisfactory.
The Stark effect in Rydberg atoms has potential applications in the areas of dipole-dipole interaction, quantum information, quantum control, and so on. Many reflevant theoretical calculations and experimental studies about the Stark effect of alkali metal and alkali earth metals have been reported, but the other atom’s Stark effect is studied still relatively less. Our goal in this paper is to reflearch the third main group atom’s Stark effect in a large electric field. First, according to the level data of gallium atom in zero-field, we obtain the quantum defects from the modified Ritz formula in each state by using a nonlinear least-squares-fitting algorithm. The quantum defects as a function of the principal quantum number are analyzed in detail. Influences of both the core polarization and the penetrating valence electron on the quantum defect are discussed according to the fitting results. Then we use the Numerov algorithm to calculate the radial wave functions of atomic gallium. Finally, the Stark structures of Rydberg states around n=7 and n=18 are numerically calculated by matrix diagonalization. Results show that at the levels above n=7 manifold states, (n+1)P is higher than nD state, and it is in contrast to the levels below the n=7 manifold states. This phenomenon is different from the usual Stark structure of alkali metal atoms, the level’s order of which does not change with the principal quantum number. The Stark levels with the identical |m| anti-cross each other, and those with different |m| cross. Our results give an important reflerence for related reflearches, and are of great significance for insight into the atomic structure and the interaction between the atomic core and the highly excited electrons.
A theory of nonhydrogenic Stark spectra based on the hydrogen atom is specialized to quasidiscrete levels. Algebraic expressions for level positions ${\ensuremath{\epsilon}}_{r}$, widths ${\ensuremath{\Gamma}}_{r}$, and oscillator strengths frF{f}_{r}^{F}frF​ are derived in terms of matrices HF{\mathit{H}}^{F}HF and hF{\mathit{h}}^{F}hF, which represent the hydrogenic density of states in a Stark field FFF. Core effects appear through zero-field quantum defects ${\ensuremath{\mu}}_{l}$ and dipole matrix elements dl0{d}_{l}^{0}dl0​. Normalized oscillator strengths f‾rF{\overline{f}}_{r}^{F}f​rF​ are defined which are independent of all dl0{d}_{l}^{0}dl0​ for $s\ensuremath{\rightarrow}p$ transitions. Isolated and interacting Stark manifolds with m=0and1m=0 \mathrm{and} 1m=0and1 are examined for systems with two nonnegligible ${\ensuremath{\mu}}_{l}$. Extensive comparisons are made with experimental Li spectra and matrix-diagonalization calculations of Zimmerman, Littman, Kash, and Kleppner [Phys. Rev. A 20, 2251 (1979); ZLKK]. For small fields F<13n5F<\frac{1}{3{n}^{5}}F<3n51​ level positions are given analytically with respect to H levels of fixed nnn; m=0m=0m=0 intensity distributions do not appear hydrogenic in Li since ${\ensuremath{\mu}}_{0}\ensuremath{\sim}\frac{1}{2}$. At F>13n5F>\frac{1}{3{n}^{5}}F>3n51​, degenerate parabolic eigenstates from different manifolds are coupled by the spherical core and avoid crossing. The upper levels disappear at m=1m=1m=1 anticrossings in Li, as observed in ZLKK. For m=0m=0m=0 the lower levels usually vanish instead. A full Stark map of calculated intensities f‾rF{\overline{f}}_{r}^{F}f​rF​ is presented for Li (m=0m=0m=0) and agrees with experiment. Pseudocrossings occur at near triple degeneracies of hydrogen Stark states. Extensions to include ls\mathrm{ls}ls coupling are indicated. Experimental ionization rates in He are analyzed in a companion paper by van de Water, Mariani, and Koch [Phys. Rev. A 30, 2399 (1984)].
With a potential model of alkali-metal atoms and B-spline expansion technique,the structure of the energy levels for Rydberg states of Rubidium is investigated.We calculated the positions and widths of anticrossing between(n+3)s and (n,k) Stark states with principal quantum number n between 16 and 25.Our results are in agreement with the experimental data.And we obtained two empirical formulas which can be used to estimate the positions of anticrossing for high Rydberg states of Rubidium in static electric field.
We present results of an experimental survey of the n=15n=15n=15 state of Na in electric fields from 0 to 4 kV/cm. Both linear and higher-order Stark effects play important roles. States with low ∣m∣|m|∣m∣ show marked differences from hydrogenic behavior, particularly in the vicinity of level crossings. Computed values for the energy levels are in good agreement with the data. The experimental method provides a simple technique for populating selected Stark or angular momentum levels of a Rydberg state.