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Physical Review Letters

Fine Structure of the nD2 Series in Rubidium near the Ionization Limit

Kenneth C. Harvey, Boris Peter Stoicheff

Published Mar 7, 1977• 107 citations
Publisher

Abstract

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 $^{2}D_{\frac{3}{2}}$ and $^{2}D_{\frac{5}{2}}$ levels of Rb for Rydberg states up to $n=85$, 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 $n<\ensuremath{\sim}25$.

DOI
10.1103/physrevlett.38.537

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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 cm\ensuremath−1{\mathrm{cm}}^{\ensuremath{-}1}cm\ensuremath−1 from the ionization limit. It is shown that the fine-structure spacing varies as neff\ensuremath−3{{n}_{\mathrm{eff}}}^{\ensuremath{-}3}neff​\ensuremath−3 for n>\ensuremath∼25n>\ensuremath{\sim}25n>\ensuremath∼25, and as a linear combination of neff\ensuremath−5{{n}_{\mathrm{eff}}}^{\ensuremath{-}5}neff​\ensuremath−5 and neff\ensuremath−3{{n}_{\mathrm{eff}}}^{\ensuremath{-}3}neff​\ensuremath−3 for n<\ensuremath∼25n<\ensuremath{\sim}25n<\ensuremath∼25.
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.
We used a tunable cw dye laser to observe Doppler-free two-photon transitions to alkali-atom Rydberg levels. Real-time signals were obtained in an ionization cell of appropriate construction. The two-photon transition wavelengths to rubidium s levels were measured up to n = 50 with better than 1 x 10(-7) absolute accuracy and can be represented to within the experimental precision by a simple function of the principal quantum number, Other related transitions and future possibilities are considered.
The multiphoton excitation of rubidium has been investigated over the 4600-6500-\AA{} wavelength region with a tunable dye-laser source having a linewidth better than 0.1 \AA{} and a space-charge ionization detector sensitive to a few ions per second. Multiphoton transitions have been observed to occur both through intermediate atomic states and through intermediate continuum states of the rubidium molecule. In the former case two-photon transitions have been observed from the 52S5^{2}S52S ground state of atomic rubidium to higher-lying n2Dn^{2}Dn2D levels for values of nnn ranging from 9 to 34 and to n2Sn^{2}Sn2S levels for values of nnn from 11 through 20. The fine-structure intervals of the n2Dn^{2}Dn2D levels for n=9toc13n=9 \mathrm{to}c 13n=9toc13 were measured together with the line-strength ratios and were found to be in good agreement with the predictions of a simple theoretical model. At the shorter wavelengths hybrid two-photon resonances were observed to be excited through resonant intermediate continuum states of Rb2{\mathrm{Rb}}_{2}Rb2​. As a result the dispersion curve for two-photon absorption in rubidium showed what appears to be resonant intermediate $p\ensuremath{\pi}(^{3}\ensuremath{\Sigma}_{u1})$ and 0g+{0}_{g}^{+}0g+​ terms dissociating to give a 5P325{P}_{\frac{3}{2}}5P23​​ atom and resulting in the strong development of features corresponding to the $5^{2}P_{\frac{3}{2}}\ensuremath{\rightarrow}n^{2}D_{\frac{3}{2},\frac{5}{2}}$ part of the diffuse series, for $n\ensuremath{\le}50$ in absorption and the $5^{2}P_{\frac{3}{2}}\ensuremath{\rightarrow}n^{2}S_{\frac{1}{2}}$ part of the sharp series. Components to 322D32^{2}D322D and 302S30^{2}S302S were recorded to a precision of 0.3 ${\mathrm{cm}}^{\ensuremath{-}1}$ and quantum defects for these previously unobserved terms were derived. The corresponding hybrid two-photon resonances involving intermediate states dissociating to give a 52P125^{2}P_{\frac{1}{2}}52P21​​ atom were not observed in the wavelength interval available in this experiment.
We have used radio-frequency spectroscopy in conjunction with a multistep optical excitation scheme involving a cw dye laser to measure the fine-structure intervals in the 62F6^{2}F62F and 72F7^{2}F72F states of Rb. We find that the fine-structure intervals $\ensuremath{\delta}w$ (in MHz) are $\ensuremath{\delta}w(6^{2}F)=\ensuremath{-}486(4)$ and $\ensuremath{\delta}w(7^{2}F)=\ensuremath{-}347.6(10)$.