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Physical Review A

Line-broadening studies of excited diatomic homoatomic and heteroatomic Rydberg molecules formed by potassium, rubidium, and cesium atoms

Cedomil Vadla, Vlasta Horvatić, Kay Niemax

Published Nov 19, 2009• 13 citations
Publisher

Abstract

Recent absorption measurements of the self-broadening of Rb principal series lines [C. H. Greene, E. L. Hamilton, H. Crowell, C. Vadla, and K. Niemax, Phys. Rev. Lett. 97, 233002 (2006)] verified the existence of minima in highly excited long-range potentials of ${\text{Rb}}_{2}$ which were predicted theoretically as bound Rydberg molecule [C. H. Greene, A. S. Dickinson, and H. R. Sadeghpour, Phys. Rev. Lett. 85, 2458 (2000)]. The present paper reports on the extension of these experimental studies to principal series lines of K broadened by K as well as Cs broadened by Cs. In addition, the broadening of some lower members of the K, Rb, and Cs principal line series due to heteroatomic interactions was investigated. The analysis of the measured satellite structures in the quasistatic line wings and their comparison to the previously published analogous data for ${\text{Rb}}^{\ensuremath{\ast}}+\text{Rb}$ system lead to the conclusion that one can expect existence of potential minima in homo- and heteroatomic alkali-metal ${A}^{\ensuremath{\ast}}+B$ systems in a wide range of principal quantum numbers, starting with K, Rb, and Cs excited to the third resonance states. The positions and strengths of the satellite structures indicate that the potential minima are due to scattering of the valence electron by ground-state perturbers.

DOI
10.1103/physreva.80.052506

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Recent absorption measurements of the self-broadening of Rb principal series lines [C. H. Greene, E. L. Hamilton, H. Crowell, C. Vadla, and K. Niemax, Phys. Rev. Lett. 97, 233002 (2006)] verified the existence of minima in highly excited long-range potentials of Rb2{\text{Rb}}_{2}Rb2​ which were predicted theoretically as bound Rydberg molecule [C. H. Greene, A. S. Dickinson, and H. R. Sadeghpour, Phys. Rev. Lett. 85, 2458 (2000)]. The present paper reports on the extension of these experimental studies to principal series lines of K broadened by K as well as Cs broadened by Cs. In addition, the broadening of some lower members of the K, Rb, and Cs principal line series due to heteroatomic interactions was investigated. The analysis of the measured satellite structures in the quasistatic line wings and their comparison to the previously published analogous data for Rb\ensuremath∗+Rb{\text{Rb}}^{\ensuremath{\ast}}+\text{Rb}Rb\ensuremath∗+Rb system lead to the conclusion that one can expect existence of potential minima in homo- and heteroatomic alkali-metal A\ensuremath∗+B{A}^{\ensuremath{\ast}}+BA\ensuremath∗+B systems in a wide range of principal quantum numbers, starting with K, Rb, and Cs excited to the third resonance states. The positions and strengths of the satellite structures indicate that the potential minima are due to scattering of the valence electron by ground-state perturbers.
Recent theoretical studies with alkali atoms A* excited to high Rydberg states predicted the existence of ultra-long-range molecular bound states. Such excited dimers have large electric dipole moments which, in combination with their long radiative lifetimes, make them excellent candidates for manipulation in applications. This Letter reports on experimental investigations of the self-broadening of Rb principal series lines, which revealed multiple satellites in the line wings. The positions of the satellites agree quantitatively with theoretically predicted minima in the excited long-range Rydberg states of Rb2.
Collisional broadening of nS Rydberg states by K, Rb, and Cs atoms is studied using the adiabatic approach for the $^{3}\mathrm{\ensuremath{\Sigma}}$ quasimolecular state and impulse approximation for all other contributions to the collisional width. The calculations are based on the use of the low-energy phase shifts for electron scattering by alkali metals obtained from ab initio close-coupling calculations and their extrapolation according to the modified effective range theory. We obtain a good agreement for the magnitude of the width with experimental data and satisfactory agreement for the oscillatory part of the width as a function of the principal quantum number. We find that the theory overestimates the amplitude of the oscillations. In the case of Cs as a perturber, the agreement with experimental data is good if we assume the existence of the low-energy 3^{3}3P resonance of ${\mathrm{Cs}}^{\mathrm{\ensuremath{-}}}$. However, recent ab initio bound-state and scattering calculations indicate the existence of the Cs (3{(}^{3}(3P) bound state rather than the resonance.
16 lines of the principal series of Cs(6 2 s 1/2 to 7-16 2 p 3/2 and 6 2 s 1/2 to 7-12 2 p 1/2 ) were investigated in absorption. Cesium vapour density was varied from 10 13 up to 10 17 cm -3 . Red asymmetries of all lines (extended red wings) were detected. This can be understood if electron transitions in the long-range interaction region follow the selection rules of molecules. It was established that the red and the blue wings of the lines each can be fitted to lorentzian profiles in small wavelength intervals. With the help of quasistatic theory the interaction constants from the long-range interaction potential Delta omega =C 3 /r 3 multiplied by the oscillator strength were determined from measurements. For all lines the ratio of C 3 (red)/C 3 (blue) was found to equal 2 in accordance with earlier theoretical calculations. In the far line wing, deviation from a lorentzian profile occurs. This was interpreted as a consequence of electron transition in the short-range region of interatomic potentials.
In addition to previous absorption measurements of Cs resonance lines, new investigations on Na, K and Rb also showed definitely that beyond symmetrical Lorentzian central parts of the lines, the stronger components of the resonance lines have blue and the weaker components red asymmetry. This behaviour can be explained by a quasistatic treatment of the self-broadening mechanism taking interatomic interaction potentials into account. But with additional data it is now possible to give a different interpretation of the origin of observed asymmetries than suggested in the previous paper on Cs resonance lines (see abstr. A5740 of 1975). The asymmetries are shown to arise from the mutual repulsion of two potential curves of the same species.
Abstract We present calculations of the photoionization (PI) cross sections of rubidium and cesium Rydberg atoms for light with wavelengths ranging from the infrared to the ultraviolet, using model potentials from Marinescu et al (1994 Phys. Rev. A 49 982). The origins of pronounced PI minima are identified by investigating the free-electron wavefunctions. These include broad PI minima in the nS to ϵP PI channels of both Rb and Cs, with free-electron energy ϵ , which are identified as Cooper minima. Much narrower PI minima in the nD to ϵF channels are due to shape resonances of the free-electron states. We describe possible experimental procedures for measuring the PI minima, and we discuss their implications in fundamental atomic physics as well as in practical applications. Measurements of PI cross sections of Rydberg atoms may serve as a sensitive probe for many-electron interactions of the Rydberg electron in the atomic core region.