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Physical Review A

Two-step stabilization of autoionizing states

J. G. Story, L. D. Van Woerkom, William E. Cooke

Published Nov 1, 1986• 9 citations
Publisher

Abstract

A two-step process using internal conversion and fluorescence to stabilize the $6{P}_{\frac{3}{2}}11d$ autoionizing state of barium has been observed. The internal conversion produces very highly excited autoionizing Rydberg states, which then emit fluorescence to produce singly excited, bound states. Inclusion of this process should bring calculations closer to agreement with recent measurements of dielectronic recombination.

DOI
10.1103/physreva.34.4508

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We have measured the relative population in the two mj{\mathit{m}}_{\mathit{j}}mj​ states of barium 6p1/2{\mathit{p}}_{1/2}p1/2​ ions produced by the autoionization of (6p3/2{\mathit{p}}_{3/2}p3/2​nd)J=MJ{)}_{\mathit{J}=\mathit{M}\mathit{J}})J=MJ​=3 states by detecting the helicity of the emitted fluorescence. These populations can be related to the relative branching ratio into the 6p1/2{\mathit{p}}_{1/2}p1/2​\ensuremath{\epsilon}d5/2{\mathit{d}}_{5/2}d5/2​ and 6p1/2{\mathit{p}}_{1/2}p1/2​\ensuremath{\epsilon}g7/2{\mathit{g}}_{7/2}g7/2​ continuum channels. Rydberg states with n=16--23 have similar branching ratios, producing approximately six times as much 6p1/2{\mathit{p}}_{1/2}p1/2​\ensuremath{\epsilon}d5/2{\mathit{d}}_{5/2}d5/2​ population as 6p1/2{\mathit{p}}_{1/2}p1/2​\ensuremath{\epsilon}g7/2{\mathit{g}}_{7/2}g7/2​ population.
We report the observation of doubly excited autoionizing Rydberg states of Sr, belonging to the configuration 5p125{p}_{\frac{1}{2}}5p21​​, nl\mathrm{nl}nl. Our procedure involves a three-step optical excitation process which incorporates Stark switching to reach higher lll states not normally accessible because of dipole selection rules. Quantum defects are reported for several 5p125{p}_{\frac{1}{2}}5p21​​, ns\mathrm{ns}ns and 5p125{p}_{\frac{1}{2}}5p21​​, nd\mathrm{nd}nd states. The lifetimes of the 5p125{p}_{\frac{1}{2}}5p21​​, ns\mathrm{ns}ns states are shown to scale as (n∗)3{({n}^{*})}^{3}(n∗)3, and the lifetimes of the 5p125{p}_{\frac{1}{2}}5p21​​, 16l16l16l states are shown to increase dramatically with increasing lll.
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.
We report the excitation of highly excited 6d52(32)nd(ns)6{d}_{\frac{5}{2}(\frac{3}{2})}\mathrm{nd}(\mathrm{ns})6d25​(23​)​nd(ns) states of barium, which lie ~5.6 eV above the first ionization limit of Ba, using two-photon excitation from the bound 6snd(ns)6snd(\mathrm{ns})6snd(ns) Rydberg states. The two-photon excitation scheme requires rather modest laser power (~0.5 mJ), and the (6d52ndj)J=4{(6{d}_{\frac{5}{2}}n{d}_{j})}_{J=4}(6d25​​ndj​)J=4​ states exhibit a sharp enhancement in the autoionization rate beyond n=25n=25n=25 which is accompanied by the onset of ejection of very-low-energy electrons ( 0.02 eV). We observe that the 6d52ndj)J=4(n25){6{d}_{\frac{5}{2}}n{d}_{j})}_{J=4}(n25)6d25​​ndj​)J=4​(n25) states predominantly autoionize to the nearly degenerate 6d(32)6{d}_{(\frac{3}{2})}6d(23​)​ state of Ba+{\mathrm{Ba}}^{+}Ba+. This result has important implications for the development of autoionization lasers and the phenomenon of dielectronic recombination.
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.