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Optics Letters

Intensity ratios of ^2D_5/2,3/2 ← ^2S doublets in the two-photon absorption spectrum of Rb and Cs

F. Arqueros, Paul E. LaRocque, Maurice S. O'Sullivan, Boris Peter Stoicheff

Published Mar 1, 1984• 15 citations
Publisher

Abstract

Absorption ratios of doublets arising from n(2)D(5/2,3/2)? n'(2)S transitions in Rb (n = 5-9, n' = 5) and Cs (n = 7-13, n' = 6) were measured by Doppler-free two-photon spectroscopy using a thermionic ion detector. The observed ratios agree with calculated values for transitions to the higher levels but differ significantly for levels n = 5 in Rb and n =7, 8 in Cs. These experiments also provide new lower bounds for the ionization potentials of Rb(2) (3.62 eV) and Cs(2) (3.682 eV).

DOI
10.1364/ol.9.000082

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Absorption ratios of doublets arising from n(2)D(5/2,3/2)? n'(2)S transitions in Rb (n = 5-9, n' = 5) and Cs (n = 7-13, n' = 6) were measured by Doppler-free two-photon spectroscopy using a thermionic ion detector. The observed ratios agree with calculated values for transitions to the higher levels but differ significantly for levels n = 5 in Rb and n =7, 8 in Cs. These experiments also provide new lower bounds for the ionization potentials of Rb(2) (3.62 eV) and Cs(2) (3.682 eV).
Doppler-free two-photon absorption spectroscopy was applied to study highly-excited D states of Rb atoms. Using a cw dye laser as an excitation source, transitions from the ground 5S state to nd 2D states (n=11-32) were observed, the ionization energy of the highest state being only 117cm-1. These D doublets are not inverted. The fine structure splittings of these states do not vary as (neff) -3, nor as n-3. The isotope shift of the 85Rb, 87Rb ground states is found to be 160±12MHz. No pressure broadening was observed for these transitions within the instrumental resolution of 15 MHz.
Two-photon, Doppler-free spectroscopy with counter-propagating beams from a cw dye laser and a new type of thermionic detector have been used to study the 2D32^{2}D_{\frac{3}{2}}2D23​​ and 2D52^{2}D_{\frac{5}{2}}2D25​​ levels of Rb for Rydberg states up to n=85n=85n=85, only 16 ${\mathrm{cm}}^{\ensuremath{-}1}$ from the ionization limit. It is shown that the fine-structure spacing varies as ${{n}_{\mathrm{eff}}}^{\ensuremath{-}3}$ for $n>\ensuremath{\sim}25$, and as a linear combination of ${{n}_{\mathrm{eff}}}^{\ensuremath{-}5}$ and ${{n}_{\mathrm{eff}}}^{\ensuremath{-}3}$ for $n<\ensuremath{\sim}25$.
Doppler-free two-photon transitions to Rydberg states in alkali metals have been recommended as a potential source of reference lines or secondary standards for wavelength calibration, because they cover a wide range of the visible spectrum.1 Observation of spectral lines for the two-photon transitions was made possible by use of a thermionic diode detector cell similar to that originally designed by Harvey.2 The Pyrex cell enclosing the diode detector and containing natural Rb was placed in a two-chamber oven so that the temperature of the cell body and that of the sidearm Rb supply could be controlled independently.
We report in this paper the principle of the calculation of the hyperfine components of a two-photon absorption line and we compare the results of the calculation with some of our expérimental results. In the first part of the paper, the two-photon transition operator is expanded on a tensorial irreductible set basis. That operator is generally the sum of two operators, one scalar and the other one quadrupolar. We deduce from it the selection rules for two-photon absorption and the formulae which permit one to calculate the intensities of the hyperfine components of a two-photon absorption line. We also report the density matrix in the excited state obtained after the two-photon excitation process, which permits one to calculate the fluorescence lines. At last we present the atomic quantities involved in the collision broadening of a two-photon absorption line. In the second part, we present the experimental hyperfine spectra obtained on the neon 21 atom for the transitions between the 3s[3/2] 2 metastable level and the 4d'[5/2] 2, 4d'[3/2] 2 and 4d[3/2] 2 excited levels. We show that the expérimental ratios between the scalar and the quadrupolar parts are very different from one transition to another. At last we compare these ratios with theoretical values obtained using the formulae of the first part. We find a good agreement between expérimental and theoretical values.
Absorption transitions between two excited optical states in ruby have been studied by comparing the absorption coefficients measured under optically pumped and unpumped conditions. The spectrum has been determined in the π-and σ-polarizations in the photon energy range from 5,500 to 45,000 cm -1 . Several absorption bands have been found which arise from the transitions from the excited states t 2g 3 2 E g and t 2g 3 2 T 1g of the Cr 3+ ion. From the locations and intensities of these bands, the terminal states of the observed transitions are assigned to the charge transfer state, the t 2g 3 2 T 2g state, and the doublet states belonging to the electron configuration t 2g 3 e g . Calculated energies between these states and the metastable states, t 2g 3 2 E g and t 2g 3 2 T 1g , are in good agreement with the peak energies of the observed absorption bands. The present experiment gives new information inaccessible by the ordinary ground state absorption measurement, such as the locations of several doublet states with the configuration t 2g 2 e g and the intensities of doublet-doublet transitions in ruby.