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Physical Review Letters

Laser resonance photoionization spectroscopy of Rydberg levels in Fr

С. В. Андреев, Vladilen S Letokhov, V.I. Mishin

Published Sep 21, 1987• 53 citations
Publisher

Abstract

We investigated for the first time the high-lying Rydberg levels in the rare radioactive element francium (Fr). The investigations were conducted by the highly sensitive laser resonance atomic photoionization technique with Fr atoms produced at a rate of about ${10}^{3}$ atoms/s in a hot cavity. We measured the wave numbers of the 7${p}^{2}$${P}_{3/2}$\ensuremath{\rightarrow}${\mathrm{nd}}^{2}$D (n=22--33) and 7${p}^{2}$${P}_{3/2}$\ensuremath{\rightarrow}${\mathrm{ns}}^{2}$S (n=23, 25--27,29--31) transitions and found the binding energy of the 7${p}^{2}$${P}_{3/2}$ state to be T=-18 924.8(3) ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$, which made it possible to establish accurately the ionization potential of Fr.

DOI
10.1103/physrevlett.59.1274

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This paper summarizes a long series of experiments that have been done on Rydberg states of Rb. The basic experimental technique that has been used is atomic-beam laser spectroscopy which allows both low-resolution and high-resolution studies. Excitation of Rydberg states is provided by single-photon absorption from a suitably frequency-doubled rhodamine 6G6G6G tunable laser. Detection is done by field ionization and ion counting. These techniques have allowed us to study the critical ionizing field, which has been found to follow classical, hydrogenic behavior closely. Rydberg states of Rb have been observed from n=28n=28n=28 up to n>100n>100n>100. High-resolution spectroscopic studies have led to measurement of the fine structure for np\mathrm{np}np levels located between n=28n=28n=28 and n=60n=60n=60, as well as the isotope shift of the ground state, $\ensuremath{\delta}\ensuremath{\nu}=(172\ifmmode\pm\else\textpm\fi{}15)$ MHz. Anomalies in the intensity ratio of the doublet $5s\ensuremath{-}np$ transitions have been observed and interpreted as relativistic effects. Perturbations by weak and strong dc electric field are reported. In the case of weak electric fields it is possible to evaluate the polarizability. In the case of strong dc electric fields, new phenomena have been observed and analyzed. We also find experimental evidence of selective photoionization in the presence of an appropriate dc electric field, which could have some applications in laser isotope separation. Finally, we give the preliminary results of an experiment on the effect of a strong nonresonant electromagnetic field on high-lying Rydberg states.
The ionization of 6sns1S06sns^{1}S_{0}6sns1S0​ Rydberg states of 138Ba^{138}\mathrm{Ba}138Ba has been investigated by high-resolution electron spectroscopy. The Rydberg states were excited by two cw dye lasers via the 6s6p1P16s6p^{1}P_{1}6s6p1P1​ level. The electron spectra show rich structure between 0.025 and 3 eV, largely attributable to collisional (Penning) ionization, photoionization, and autoionizing transitions. The first process might be interpreted as superelastic scattering of the Rydberg electron by optically pumped Ba(6s6p1P1)\mathrm{Ba}(6s6p^{1}P_{1})Ba(6s6p1P1​) or Ba(6s5d1D2)\mathrm{Ba}(6s5d^{1}D_{2})Ba(6s5d1D2​) atoms.
Francium is the least studied of the alkali atoms because it has no stable isotopes. We have performed precision spectroscopy on cold Fr atoms in a magneto optical trap. We have determined the location of the first two excited states of the S series by two-photon spectroscopy. We have measured the lifetimes of the 7p levels with a precision better than 0.5%. Our measurements test the many-body perturbation theory ab initio calculations of the dipole matrix element to very high accuracy in this relativistic alkali.
We present lifetime measurements of the 7D3/2{7D}_{3/2}7D3/2​ and 7D5/2{7D}_{5/2}7D5/2​ levels of Fr. We use a time-correlated single-photon counting technique on a sample of 210Fr{}^{210}\mathrm{Fr}210Fr atoms confined and cooled in a magneto-optical trap. The upper state of the 7P3/2{7P}_{3/2}7P3/2​ trapping transition serves as the resonant intermediate level for two-photon excitation of the 7D7D7D states. A probe laser provides the second step of the excitation, and we detect the decay of the atomic fluorescence. Our measurements help extend the knowledge of this class of atomic wave functions in which correlation effects are very significant. We measure lifetimes of $73.6\ifmmode\pm\else\textpm\fi{}0.3 \mathrm{ns}$ and $67.7\ifmmode\pm\else\textpm\fi{}2.9 \mathrm{ns}$ for the 7D3/2{7D}_{3/2}7D3/2​ and 7D5/2{7D}_{5/2}7D5/2​ levels, respectively.
We present lifetime measurements of the 7p2P3/2{7p}^{2}{P}_{3/2}7p2P3/2​ and 7p2P1/2{7p}^{2}{P}_{1/2}7p2P1/2​ levels of Fr. We use a time-correlated single-photon counting technique on a cold sample of 210Fr{}^{210}\mathrm{Fr}210Fr atoms in a magneto-optic trap. We excite the atoms with the trapping and repumping beams of the magneto-optic trap and detect the decay of the atomic fluorescence. The results are a precision experimental test of the atomic many-body perturbation theory applied to the heaviest alkali metal. The lifetime results are 21.02(11) ns and 29.45(11) ns for the 7p2P3/2{7p}^{2}{P}_{3/2}7p2P3/2​ and 7p2P1/2{7p}^{2}{P}_{1/2}7p2P1/2​ levels, respectively. This gives a line strength ratio S1/2{\mathcal{S}}_{1/2}S1/2​/S3/2{\mathcal{S}}_{3/2}S3/2​ of 0.526(3) for these levels in Fr. To study sources of systematic errors we measure the lifetimes of 5p2P3/2{5p}^{2}{P}_{3/2}5p2P3/2​ and 5p2P1/2{5p}^{2}{P}_{1/2}5p2P1/2​ in stable 87Rb{}^{87}\mathrm{Rb}87Rb and obtain 26.20(9) ns and 27.64(4) ns, respectively.