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Journal of the Optical Society of America B

Limitation of sequential laser excitation for double-Rydberg autoionizing states of barium and quantum-defect approach

Jacques Boulmer, Pierre Camus, J. M. Lecomte, P. Pillet

Published Oct 1, 1988• 15 citations
Publisher

Abstract

The limitations of methods of excitation and analysis of double-Rydberg states of neutral barium atoms are discussed. Excitation spectra of the type 6snd → 9dn′d are studied and interpreted in a two-channel quantum-defect model for n ≥ 15. No resonance is observed for n < 15, which fixes the limit of the possibilities of the sequential laser excitation. Similar behavior is observed for excitation spectra 6snp → 26dn′p and 6snp → 27sn′p for n < 39.

DOI
10.1364/josab.5.002199

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Jacques Boulmer, Pierre Camus, P. Pillet

Methods of excitation and analysis of double-Rydberg states of the neutral barium atom are discussed. Spectra of 9dn′d double-Rydberg series of barium are studied and interpreted in a two-channel quantum-defect model. An example of stabilization for the 9d5/227d state is shown. We propose a new investigative method for Rydberg levels of the Ba+ ion that is based on a microwave-ionization process coupled with a double time-of-flight mass spectrometer. This novel setup permits us to obtain initial experimental evidence of highly excited double-Rydberg states, 26dn′p and 27sn′p (n′ ≳ 45), of the barium atom.

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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.

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Chinese journal of atomic and molecular physics•Jan 1, 1990•0 citations

Novel Experimental Method in the Study of Double Rydberg States by Laser Resonance Excitation

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We describe a novel experimental method by introducing sequential ionization with a pulsed and a strong constant electric field in a time-of-flight mass spectrometer. This method is applied to study laser-excited double Rydberg states of neutral ytterbium atom, with the ionic resonance background in the spectrum of the double Rydberg states of Yb being greatly suppressed.

中国激光(英文版)•Jan 1, 1997•0 citations
The limitations of methods of excitation and analysis of double-Rydberg states of neutral barium atoms are discussed. Excitation spectra of the type 6snd → 9dn′d are studied and interpreted in a two-channel quantum-defect model for n ≥ 15. No resonance is observed for n < 15, which fixes the limit of the possibilities of the sequential laser excitation. Similar behavior is observed for excitation spectra 6snp → 26dn′p and 6snp → 27sn′p for n < 39.
Methods of excitation and analysis of double-Rydberg states of the neutral barium atom are discussed. Spectra of 9dn′d double-Rydberg series of barium are studied and interpreted in a two-channel quantum-defect model. An example of stabilization for the 9d5/227d state is shown. We propose a new investigative method for Rydberg levels of the Ba+ ion that is based on a microwave-ionization process coupled with a double time-of-flight mass spectrometer. This novel setup permits us to obtain initial experimental evidence of highly excited double-Rydberg states, 26dn′p and 27sn′p (n′ ≳ 45), of the barium atom.
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.
Laser-induced autoionization, a form of forced autoionization, is discussed. Highly excited atomic Rydberg states generally have a small cross section for photoionization due to their small overlap with the nucleus. The cross section for photoionization can be strongly enhanced if the Rydberg series is perturbed by an atomic state with a relatively large cross section for photoionization. The photoionization dynamics of such a perturbed Rydberg system shows strong similarities to that of an autoionizing Rydberg series. For intense laser pulses, which strongly couple the perturber to the continuum, the photoionization rate is limited by the coupling between the Rydberg states and the perturber or, in other words, the autoionization rate. The model describing this ionization dynamics is applied to the barium 6snd(1,3{(}^{1,3}(1,3D2{\mathit{D}}_{2}D2​) state which is perturbed by the 5d7d(1{(}^{1}(1D2{\mathit{D}}_{2}D2​) state. The calculations show good agreement with experimental results of photoionization of barium Rydberg states with subpicosecond laser pulses of light of 620 nm in wavelength.
In the study of Yb atomic Rydberg states, new members of 6sns 1 S 0 series for n=23, 24, 66-116 and 6snd 1 D 2 series for n=81-114 were observed. The data are in excellent agreement with the MQDT analysing results. The autoionizing Rydberg series 6p 1 2 /n's ( 1/2 , 1/2 ) 1 0 were investigated by three-step laser excitation. The ICE model was used to explain the experimental spectrum, and it has been proved to be suitable for describing the excitation of the autoionizing Rydberg states with a weakly-excited core.