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Le Journal de Physique Colloques

OBSERVATION OF THE 5dnl EVEN DOUBLY-EXCITED STATES IN NEUTRAL BARIUM USING TWO-STEP OPTOGALVANIC SPECTROSCOPY

Pierre Camus, M. Dieulin, A. El Himdy

Published Nov 1, 1983• 0 citations
Publisher

Abstract

Even parity levels of neutral barium above the 6s ionization limit have been investigated by using a two-step pulsed laser excitation associated with optogalvanic detection of the optical resonances. From the metastable states, 5d6s, populated by a d.c. discharge in a heat-pipe vapour, the doubly excited 5dnl Rydberg series with J values ranging from 0 to 5 and the 6p2 1S0 levels have been observed in the continuum between the first 6s and the second 5d ionization limits of Ba I.

DOI
10.1051/jphyscol:1983724

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Technique to study Rydberg states by multiphoton ionization spectroscopy

R. D. Verma, Alak Chanda

A new technique to study the Rydberg states of the barium atom has been developed. In this technique a multiphoton ionization signal is detected by selective excitation of the ground-state ion (6s) to an excited state (6p), which results in a collimated amplified spontaneous emission signal at the 6p → 5d transition of Ba+. Discrete Rydberg states, 6snl (l = 0, 2), as well as autoionizing Rydberg states, 5dnl (l = 0, 2) and 6pnl (l = 0, 2) are observed by this novel but simple method.

Journal of the Optical Society of America B•Jan 1, 1988•6 citations
Even parity levels of neutral barium above the 6s ionization limit have been investigated by using a two-step pulsed laser excitation associated with optogalvanic detection of the optical resonances. From the metastable states, 5d6s, populated by a d.c. discharge in a heat-pipe vapour, the doubly excited 5dnl Rydberg series with J values ranging from 0 to 5 and the 6p2 1S0 levels have been observed in the continuum between the first 6s and the second 5d ionization limits of Ba I.
An optogalvanic detection scheme, in conjunction with a single-step pulsed laser excitation has been used to measure the energy of even parity Rydberg levels in krypton. The excitation scheme starts from the 5s(3/2)2 and 5s'(1/2)0 metastable states, which have been populated in a He-Kr discharge tube. Measured energies were compared to either calculated or previously measured values. Calculated energies were obtained with the Rydberg formula using quantum defects extrapolated from the known low-lying levels. Keywords include: Krypton, Rydberg atoms, Atomic spectra, Optogalvanic spectroscopy.
We present new experimental data on the highly excited levels in mercury using the optogalvanic detection technique in conjunction with a dc discharge cell. The collisionally populated 6s6p 3P2 metastable level has been used as an intermediate level to access the Rydberg states using a frequency-doubled dye laser covering the wavelength region between 370 and 249 nm. The optogalvanic data reveal 6sns 3S1(13≤n≤50), 6snd 2D1(6≤n≤18), 6snp 3D1(6≤n≤14), 6snd 3D2(6≤n≤15), and 6snd 3D3(6≤n≤59) Rydberg series. The 6sns 3S1 and 6snd 3D3 Rydberg series to such a high n value have been reported for the first time. In addition, collisionally induced parity-forbidden transitions 6snp 3P1(44≤n≤50) have been detected.
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.
We report the observation of unusual doubly excited states of barium: Ba (5dj, 21c). One of the valence electrons of Ba is prepared in an oriented circular Rydberg state (n = 21, l = m = 20, denoted 21c) by the adiabatic crossed-fields method. The other electron is excited to a 6pj state which decays radiatively to a 5dj metastable level. The measured autoionization lifetime of Ba (5d5/2, 21c) is T ~ 1 μ s , whereas for Ba (5d3/2, 21c), τ is estimated to be longer than 400 μs. This very large difference of lifetimes between the fine-structure states of the inner electron has been analysed.
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.