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Physical Review A

High-resolution studies on bound odd-parity Rydberg states in Ba I

E. R. Eliel, W. Hogervorst

Published Jun 1, 1983• 22 citations
Publisher

Abstract

A study of the detailed structure of the bound odd-parity Rydberg states of barium has been undertaken using a cw dye laser in combination with an atomic beam. Special attention has been paid to the $6snf$ configurations, of which the hyperfine structure has been analyzed in terms of a small set of parameters. In addition to an effective Slater-exchange integral, an effective spin-orbit interaction, and a contact hyperfine parameter, a new parameter representing two-body magnetic effects, has been introduced. The introduction of this new parameter is discussed in some detail. Good agreement between the calculated and experimental hyperfine energies is achieved in this way.

DOI
10.1103/physreva.27.2995

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Stark spectra of barium Rydberg states above the classical field-ionization limit have been recorded at high density of states employing high-resolution laser spectroscopy. The spectra, taken at a binding energy of about \ensuremath{\varepsilon}\ensuremath{\approxeq}-55 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ with respect to zero-field threshold and at electric-field strengths F\ensuremath{\approxeq}100 V/cm exhibit dramatic variations in line profiles with increasing external field strength. The WKB quantum-defect theory of the Stark effect of nonhydrogenic atoms was used to analyze the recorded spectra, and excellent agreement between measured and calculated line profiles was achieved. Core-induced coupling of closed and open hydrogenic Stark channels was found to contribute dominantly to the linewidth of the recorded Stark resonances. In addition, a reformulation of this theory by McNicholl, Ivri, and Bergeman (unpublished) in terms of a configuration-interaction model was employed to analyze a particular avoided crossing of several Stark components. In this way recorded line profiles were parametrized within a limited model to obtain resonance energies, linewidths, and Fano q parameters.

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A study of the detailed structure of the bound odd-parity Rydberg states of barium has been undertaken using a cw dye laser in combination with an atomic beam. Special attention has been paid to the 6snf6snf6snf configurations, of which the hyperfine structure has been analyzed in terms of a small set of parameters. In addition to an effective Slater-exchange integral, an effective spin-orbit interaction, and a contact hyperfine parameter, a new parameter representing two-body magnetic effects, has been introduced. The introduction of this new parameter is discussed in some detail. Good agreement between the calculated and experimental hyperfine energies is achieved in this way.
Odd-parity barium Rydberg states have been populated by stepwise excitation via M1-E1 and E2-E1 transitions, starting from the 6s2 1S0 ground state. Using two cw dye ring lasers and employing thermionic detection, Doppler-free spectra of 6snp 1,3P and 6snf 1,3F Rydberg states have been recorded with excellent signal/noise ratios. A systematic study of the hyperfine structure of 6snp 1P1 Rydberg states has been carried out. Between n=20 and n=23 a resonance in singlet-triplet mixing occurs caused by configuration interaction with the 5d8p 1P1 perturbing state, located close to the first ionization limit. Our results are in disagreement with an existing multichannel quantum defect analysis of this series. The singlet-triplet mixing of 6snp 1P1 and 6snd 1D2 Rydberg series is compared.
High Rydberg levels of ytterbium were studied in a beam of metastable atoms. Levels of the series 4f14^{14}14 6snsnsnd were populated from the metastable 4f14^{14}14 6s 6p 3^33Po_oo​ level by means of the U.V. light of a frequency-doubled single-mode dye laser and detected using the field ionization technique. The critical ionization fields FcF_cFc​ of the levels 4f14^{14}14 6snsnsnd 3^33D1_11​ (24 ≤ n ≤ 57) were measured and found to obey the saddle point law (FcF_cFc​ = (16 n∗4n^{*4}n∗4)−1^{-1}−1). The hyperfine structures of the odd isotopes were investigated. They are very peculiar due to the fact that the hyperfine interaction is of the same order of magnitude as (or even for the highest nnn values, much more important than) the spin-orbit and electrostatic interactions. A theoretical account of the observed structures using the Slater-Condon parametric method is given. The relative influence of the excited (nnnd) and of the non-excited (6s) optical electron could thus be studied. Furthermore the influence of a valence level perturbing only the odd isotopes components for nnn = 26 was demonstrated.
The MQDT of hyperfine structure is greatly simplified in extremely high Rydberg states. A four (or three)-channel quantum defect model is derived for the hyperfine structure of extremely high Rydberg states of msnd configuration in odd alkaline-earth isotopes, in which the transformation matrix U i(F)i' is given analytically except for one parameter which measures the mixing of singlet 1 D 2 and triple 3 D 2 induced by spin-orbit interaction in even isotopes, and in which the four eigen quantum defects mu i' (i'=1, 2, 3, 4) are related to the quantum defects of the fine structure in even isotopes by mu i' =mod( delta i' ). This model has been used to interpret the observed sublevel structure of 5snd (n>100) configurations in 87 Sr. An excellent agreement between the theoretical and experimental results was achieved.
The even-parity spectra of strontium and barium are very complex due to strong perturbation by several doubly excited configurations and this also increases discrepancies between theory and experiment in accurate level assignment and energy level and atomic structure data, particularly for the spectra of highly excited atoms and their behaviour in external fields and collisional processes which are of fundamental importance in the emerging applications in physics of cold atoms, quantum computing, precision atomic clocks and in the crossed-field problem. This thesis presents results from an experimental study to improve and extend the previously published observations in the two-photon spectra of the high-lying Rydberg states of SrI and Bal placed under a variety of test conditions such as external fields, collisions etc. Orthogonal excitation of a novel atomic jet in a purpose-built heat-pipe setup using a Xenon Chloride excimer laser pumped tunable narrow bandwidth dye laser and high sensitivity space-charge ionization in thermionic diode with complimentary optical detection was used for measurements. Presented are the two-photon spectra covering the dye laser wavelength (air) range of 460 - 425 nm for strontium and 495 - 467 nm for barium by which the J = 0,2 even-parity Rydberg series and autoionizing resonances just above the ionization limits labeled as; (4d2+5p2) 1D2 in strontium and 5d5f2p1 in barium were observed. Original new energy level values are presented with substantial extension to the data in the literature for even-parity Rydberg series: Sr I: 5sns 1S0 (12 < n < 46), 5snd 3D2 (9 < n < 47) and 5snd 1D2 (9 < n < 82) Ba I: 6sns 1S0 (13 < n < 68), 6snd 3D2 (11 < n < 46) and 6snd 1D2 (11 < n < 88) New observation of certain anomalies including a Stark shift reversal effect and zero-field thermionic diode detection with remarkable sensitivity preserving all spectral features of Rydberg states is also presented. Controlled configuration mixing by exploiting electric field and collisions has allowed new observations for the two-photon forbidden odd-parity Rydberg series of SrI: 5s2 1S0 -> 5snp 1P1o (32 < n < 46) and 5s2 1S0 -> 5snf 1F30 (29 < n < 44) Extensive study of collision involving Rydberg atoms with neutral rare gas atoms has allowed to obtain new data for shift and broadening rates for Sr I series: 5sns 1S0 and 5snd 1,3D2 in the perturbed region which clearly exhibit Ramsauer effect. Collisional evolution of a remarkably broad resonance, labeled as 4d2 1G4, also exhibiting Ramsauer effect, is presented besides new level data for strontium 4d2 3PJ states accessed by two distinct processes- direct two-photon excitation and single-photon sequential excitation. Furthermore, the thesis presents the results of a novel experimental technique involving time-resolved gated pulsed field detection technique (GPT) employed for the first time to examine the time decay of Rydberg atoms yielding their effective lifetimes.
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.
Stark spectra of barium Rydberg states above the classical field-ionization limit have been recorded at high density of states employing high-resolution laser spectroscopy. The spectra, taken at a binding energy of about \ensuremath{\varepsilon}\ensuremath{\approxeq}-55 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ with respect to zero-field threshold and at electric-field strengths F\ensuremath{\approxeq}100 V/cm exhibit dramatic variations in line profiles with increasing external field strength. The WKB quantum-defect theory of the Stark effect of nonhydrogenic atoms was used to analyze the recorded spectra, and excellent agreement between measured and calculated line profiles was achieved. Core-induced coupling of closed and open hydrogenic Stark channels was found to contribute dominantly to the linewidth of the recorded Stark resonances. In addition, a reformulation of this theory by McNicholl, Ivri, and Bergeman (unpublished) in terms of a configuration-interaction model was employed to analyze a particular avoided crossing of several Stark components. In this way recorded line profiles were parametrized within a limited model to obtain resonance energies, linewidths, and Fano q parameters.