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Physical Review Letters

High-Resolution Electron Spectroscopy of Laser-Excited Ba Rydberg Atoms

Herbert H. Rinneberg, Jörg Neukammer, U. Majewski, Gerd Schönhense

Published Oct 24, 1983• 15 citations
Publisher

Abstract

The ionization of $6sns^{1}S_{0}$ Rydberg states of $^{138}\mathrm{Ba}$ has been investigated by high-resolution electron spectroscopy. The Rydberg states were excited by two cw dye lasers via the $6s6p^{1}P_{1}$ 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 $\mathrm{Ba}(6s6p^{1}P_{1})$ or $\mathrm{Ba}(6s5d^{1}D_{2})$ atoms.

DOI
10.1103/physrevlett.51.1546

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Physical Review A•Jun 1, 1986•10 citations
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.
High-resolution three-photon laser spectroscopy has been performed for the first time to gain new spectroscopic information. Starting from the $6{s}^{2}^{1}S_{0}$ ground state of Yb, 6s15p1,3P16s15p^{1,3}P_{1}6s15p1,3P1​ Rydberg states were populated by two-photon-resonant, three-photon absorption via the 6s7s1S06s7s^{1}S_{0}6s7s1S0​ intermediate level. As a result of two-photon line narrowing Doppler-free spectra, showing well resolved isotope shifts and hyperfine structures, were obtained. From the hyperfine coupling constants 171,173A(1P1)^{171,173}A(^{1}P_{1})171,173A(1P1​) the singlet-triplet mixing was derived.
Using transverse laser excitation of a single collimated atomic sodium beam in combination with an efficient electron spectrometer, we have studied collisional (= Penning) and photoionization processes involving the laser-excited Na(3 p 3/2 ) and Na(3 d 5/2 ) atoms. As a result of our high electron energy resolution (6 meV) we have for the first time been able to measure the polarization-dependent lineshapes of the Penning electron spectra for collisions between two laser-excited atoms and to reliably separate overlapping contributions due to Penning and photoionization.
We demonstrate an experimental technique that selects the nuclear spin I=0 isotope 138Ba^{138}\mathrm{Ba}138Ba for spectroscopic measurements from a beam of natural barium containing seven stable isotopes. A cw dye laser is used to optically pump the I=3/2 isotopes 135Ba^{135}\mathrm{Ba}135Ba and 137Ba^{137}\mathrm{Ba}137Ba into the metastable 6s5d 1^{1}1D2{\mathit{D}}_{2}D2​ and 3^{3}3D1,2{\mathit{D}}_{1,2}D1,2​ levels via the 6s6p 1^{1}1P1{\mathit{P}}_{1}P1​ excited state, leaving nearly pure 138Ba^{138}\mathrm{Ba}138Ba in the ground state. Photoionization spectra of the excited 5d6p 3^{3}3D1{\mathit{D}}_{1}D1​ even isotope state recorded with optical pumping of 135Ba^{135}\mathrm{Ba}135Ba and 137Ba^{137}\mathrm{Ba}137Ba to the metastable levels are essentially devoid of forbidden features associated with the hyperfine interaction in the odd isotopes.
The production of very-high-nnn ($n\ensuremath{\sim}300$--500) strontium Rydberg atoms is explored using a crossed-laser-atom-beam geometry. nnn1S0{}^{1}{S}_{0}1S0​ and nnn1D2{}^{1}{D}_{2}1D2​ states are created by two-photon excitation via the 5s5p5s5p5s5p 1P1{}^{1}{P}_{1}1P1​ intermediate state using radiation with wavelengths of $\ensuremath{\sim}$461 and $\ensuremath{\sim}$413 nm. Rydberg atom densities as high as $\ensuremath{\sim}3\ifmmode\times\else\texttimes\fi{}{10}^{5}$ cm${}^{\ensuremath{-}3}$ have been achieved, sufficient that Rydberg-Rydberg interactions can become important. The isotope shifts in the Rydberg series limits are determined by tuning the 461-nm light to preferentially excite the different strontium isotopes. Photoexcitation in the presence of an applied electric field is examined. The initially quadratic Stark shift of the nnn1P1{}^{1}{P}_{1}1P1​ and nnn1D2{}^{1}{D}_{2}1D2​ states becomes near-linear at higher fields and the possible use of n1D2n{}^{1}{D}_{2}n1D2​ states to create strongly polarized, quasi-one-dimensional electronic states in strontium is discussed. The data are analyzed with the aid of a two-active-electron (TAE) approximation. The two-electron Hamiltonian, within which the Sr2+{}^{2+}2+ core is represented by a semi-empirical potential, is numerically diagonalized allowing the calculation of the energies of high-nnn Rydberg states and their photoexcitation probabilities.
Three-photon ionization spectra of Ba were studied which result from two-photon resonances between the 6s2{s}^{2}s2 1{\mathrm{}}^{1}1S0{S}_{0}S0​ ground state and the 6snd J=2,6s(n+1)s 1{\mathrm{}}^{1}1S0{S}_{0}S0​ (16\ensuremath{\le}n40) Rydberg states and 5d7d 1{\mathrm{}}^{1}1D2{D}_{2}D2​,3{\mathrm{}}^{3}3P0{P}_{0}P0​,2 perturber states. A tunable laser with field strength ${10}^{\mathrm{\ensuremath{-}}(4\mathrm{\ensuremath{-}}5)}$ a.u. was used to drive the excitation in a low-density atomic beam (n\ensuremath{\lesssim}3\ifmmode\times\else\texttimes\fi{}108{10}^{8}108 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$). Resonant line shapes were systematically studied as a function of light polarization and intensity. Studies with linearly polarized light find all resonant line shapes manifest the same peak shift and asymmetry which is traced to the ac Stark shift of the ground state. The resonant peak height, shift, and linewidth scale linearly with light intensity which is accounted for with a rate-equation formulation.For the case of circular polarization, a distinct minimum of ionization occurs between each J=2 doublet of the 6snd series. One level (generally 3D2^{3}\mathrm{D}_{2}3D2​) is significantly broadened in comparison to the laser linewidth (0.1 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$) with increasing intensity while its sister level remains narrow (\ensuremath{\sim}0.2 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$). Further, light shifts of the 3D2^{3}\mathrm{D}_{2}3D2​ states are generally \ensuremath{\gtrsim}1 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ to the red while shifts of 1D2^{1}\mathrm{D}_{2}1D2​ states are negligible. This behavior switches for the n=27 doublet. Lastly, the dynamic shifts are not quadratic with the field strength. These effects are attributed in part to cancellation due to channel interference and a two-photon Raman process which mixes each J=2 doublet. These processes act in conjunction with the ac Stark effect to produce the observed profile behavior. The shifts and coupling of the excited states are attributed to the influence of the 6pnd ${J}^{\ensuremath{\pi}}$${=3}^{\mathrm{\ensuremath{-}}}$ autoionization series and are shown to be sensitive to the singlet-triplet mixing coefficient \ensuremath{\beta} of the J=2 doublets. A perturbation analysis is introduced which accounts for the salient features of the data, although it does not include bandwidth and saturation effects. Calculations of light shifts of the 6snd J=2 levels based on this analysis require \ensuremath{\beta} be modified from previous assignments based on hfs measurements for n in the vicinity of the 5d7d 1{\mathrm{}}^{1}1D2{D}_{2}D2​ perturber.