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Journal of Physics B Atomic Molecular and Optical Physics

Collisional broadening of Rydberg atom transitions by rare gas perturbers

Megan E Henry, Roger M. Herman

Published Jan 10, 2002• 7 citations
Publisher

Abstract

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.

DOI
10.1088/0953-4075/35/2/313

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Journal of Physics B Atomic and Molecular Physics•Nov 28, 1984•41 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 broadening and shift of two-photon $S\ensuremath{-}S$ transitions (e.g., in alkali-metal atoms perturbed by rare gases) are shown to be readily calculable. These calculations employ (a) newly available expressions for alkalimetal-rare-gas long-range potential coefficients C6{C}_{6}C6​, C8{C}_{8}C8​, and C10{C}_{10}C10​; and (b) the (herein discussed) appropriate form of impact theory (particularly simple since only a single potential curve is involved and inelastic processes are not usually important). It is demonstrated in particular that the influence of C8{C}_{8}C8​ and C10{C}_{10}C10​ terms on the broadening and shift is significant though not dominant. Comparison with recent experimental data on the Na-rare-gas pairs shows reasonable agreement for the heavy rare gases.
Our recent treatment [Phys. Rev. A 18, 1066 (1978)] of the broadening and shift of alkali-metal-atom two-photon $S\ensuremath{-}S$ transitions is applied to the Na $3S\ensuremath{-}\mathrm{nS}$ transitions ($n=6\ensuremath{-}9$) perturbed by Ar, Kr, and Xe rare gases. Comparison with recent experimental data [A. Flusberg et al., Phys. Rev. A 19, 1607 (1979)] on the Na-Ar pair for $n\ensuremath{\le}7$ shows good agreement. However, for transitions to n>8n>8n>8 the calculated pressure effects no longer agree well with experimental data; presumably the pressure effects cannot be adequately described by a simple two-body long-range impact theory.
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.