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Optics Communications

On the self-shift and broadening of doppler-free Rydberg 2S spectral lines in alkali atoms

Yitzhak Rabin, Frank Rebentrost

Published Jan 1, 1982• 13 citations
Publisher
DOI
10.1016/0030-4018(82)90307-8

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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 $^{2}\mathrm{S}$ and $^{2}\mathrm{D}$ states (with n\ensuremath{\sim}10--40) for ${\mathrm{Rb}}^{\mathrm{*}\mathrm{*}}$+Rb and ${\mathrm{K}}^{\mathrm{*}\mathrm{*}}$+K, and of $^{2}\mathrm{S}$ states (with n=14--29) for ${\mathrm{K}}^{\mathrm{*}\mathrm{*}}$+Rb. Large oscillations are observed in both broadening and shift rates for n\ensuremath{\sim}20--30 in all series except for the $^{2}\mathrm{D}$ series in ${\mathrm{Rb}}^{\mathrm{*}\mathrm{*}}$+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.

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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.

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Pressure Shift and Broadening of Alkali Rydberg States.

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•Jan 1, 1986•0 citations
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.
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.