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AIP conference proceedings

Theory of quantum oscillations in self-broadening of 4[sup 2]S-n[sup 2]S Rydberg transitions in potassium

R. M. Herman, M. E. Henry

Published Jan 1, 1997• 0 citations
Publisher

Abstract

A pseudohamiltonian impact theory for describing Rydberg transition line shapes is proposed. Preliminary results give lineshapes in reasonable agreement with experiment, including the quantum oscillations in alkali self broadening and shifting, and rare gas broadening.
DOI
10.1063/1.51855

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Physical Review A•Jan 1, 1987•35 citations
In this paper we present the results and discuss the applicability of an impact theory of lineshapes, developed by Henry and Herman for the pressure-induced broadening and shifting of transitions from the ground state to various Rydberg states of alkalis, to the situation in which the perturbing atoms are ground-state rare gas atoms. This theory, which has successfully described the collisional broadening of Rydberg states by alkali atoms, can without major alterations predict the widths and shifts of Doppler-free two-photon transitions to n S and n D states of Rb and Na, 6⩽ n ⩽30, perturbed by He, Ne, Ar, Kr and Xe. The results in all cases show reasonable agreement with experiment, with the transitions to Na**( n D) states being somewhat less satisfactory than the others.
A theory is developed that allows a qualitative explanation and quantitative calculation of the widths and shifts of the two-photon Doppler-free transitions from the ground states of alkali atoms to Rydberg n 2 S and n 2 D states. The widths and shifts result from collisions between Rydberg atoms and ground-state alkali atoms, either of the same or of other species. The collisions are represented by means of a pseudopotential that is a function of theoretically calculated free-electron elastic scattering resonant and nonresonant phase shifts, which depend upon the Rydberg electron momentum. The momentum, in turn, is correlated with the electronic position within the Rydberg atom. This theory assumes classical straight-line trajectories and takes into consideration the multicollisional nature of the Rydberg-electron-perturbing-atom interaction within the Rydberg atom. Impact theory calculations of the linewidths and shifts for K**( n S)-K, K**( n S)-Rb, Rb**( n S)-Rb, Rb**( n S)-K, K**( n D)-K, K**( n D)-Rb, Rb**( n D)-Rb and Rb**( n D)-K show substantial agreement with experiment for 10⩽ n ⩽40.
The theory of impact broadening of the isolated spectral lines of the Rydberg atomic series perturbed by neutral particles is developed within the framework of the impulse approximation. The analysis of the broadening process is based on the consideration of the inelastic nl to n' transitions between highly excited states of the Rydberg atom. The role of the potential and resonance scattering of the quasifree electron by a perturbing particle in the impact broadening of the Rydberg nl levels is investigated. It is shown that the general expressions for the broadening cross sections presented in this paper contain the results of asymptotic Alekseev and Sobel'man theory (1965) as special cases. Both elastic and inelastic scattering contributions of the perturber by the parent core of Rydberg atom to the broadening cross sections are also considered within the framework of the 'shake' model. The results obtained are used for a quantitative explanation of experimental data on the broadening of Rydberg atomic levels perturbed by alkali-metal atoms. The energies and widths of the 3 P resonances on the quasidiscrete levels of the negative K - and Rb - ions are determined.
The author obtains expressions for Rydberg level broadening and shift cross sections and rates suitable for elastic collisions of ground-state rare-gas atoms with Rydberg atoms. The semiclassical impact broadening theory is used. The interaction of a Rydberg atom with a rare-gas atom is approximated by the superposition of polarisation potentials and the Fermi pseudopotential. It is shown that similar expressions for the broadening and shift cross sections due to the perturber-Rydberg-electron interaction can be obtained in the JWKB approximation for the Rydberg-electron wavefunctions and for the square-well model potential. Consequently the shift and width of the Rydberg level are not very sensitive to the shape of the potential but only to its normalisation. Expressions for the shift and width in the square-well potential approximation suitable in the high-density limit of the perturbing atoms are obtained. Limits of the applicability of the expressions for the broadening and shift cross sections are discussed. Calculated broadening and shift rates agree well with experimental results for the broadening and shift of Rydberg levels with small, medium and large principal quantum numbers by all rare gases excepting neon.
The technique of Doppler-free two-photon spectroscopy was used to measure rates for line broadenings and frequency shifts of Rydberg levels with pressure. Measurements were made of spectra of 2S^{2}\mathrm{S}2S and 2D^{2}\mathrm{D}2D states (with n\ensuremath{\sim}10--40) for Rb∗∗{\mathrm{Rb}}^{\mathrm{*}\mathrm{*}}Rb∗∗+Rb and K∗∗{\mathrm{K}}^{\mathrm{*}\mathrm{*}}K∗∗+K, and of 2S^{2}\mathrm{S}2S states (with n=14--29) for K∗∗{\mathrm{K}}^{\mathrm{*}\mathrm{*}}K∗∗+Rb. Large oscillations are observed in both broadening and shift rates for n\ensuremath{\sim}20--30 in all series except for the 2D^{2}\mathrm{D}2D series in Rb∗∗{\mathrm{Rb}}^{\mathrm{*}\mathrm{*}}Rb∗∗+Rb. Overall rates for broadening and shift are compared with a theory based on the ``free-electron'' model. The observed oscillations are inconsistent with theories based on the resonance scattering of the Rydberg electron by the perturbing atom. A possible alternative mechanism related to interference in l-mixing collisions is suggested.