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Optics Letters

Ionization studies in laser-excited alkaline-earth vapors

J.P. Hermann, James J. Wynne

Published Jun 1, 1980• 9 citations
Publisher

Abstract

We report on the time behavior of ionization signals produced by laser excitation of Ca and Ba atomic vapor to high-Rydberg states. A space-charge-limited thermionic diode detector shows a long-lived (>I-msec) ionization signal. However, optical detection of atomic ions (Ca+, Ba+) shows that these species live for much shorter times (<100 microsec). These results, in conjunction with published results on mass-spectrometric studies of high-density atomic beams, suggest that our ionization signal is primarily due to molecular species (Ca2+, Ba2+). We also observed optically pumped amplified spontaneous emission and stimulated electronic Raman scattering in Ca+ and Ba+.

DOI
10.1364/ol.5.000236

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In this work radiative properties of neutral elements with one or two electrons outside closed subshells have been investigated. Using laser techniques in connection with atomic beams selective excitation of Rydberg states was performed. Most of the studied states were populated with two-step excitation. Some states were reached directly from the ground state or from a metastable state and occasionally two-photon absorption was used. The excitation sometimes involved the use of frequency-doubling and Raman- shifting techniques. By time-resolved detection of the decay light from an excited state, primarily information on the radiative lifetime is obtained. With two different experimental arrangements radiative lifetimes in several Rydberg states have been determined. Using the quantum-beat technique time-resolved detection also provides information on energy splittings. This technique was used to measure hyperfine-structure splittings.To obtain information about hyperfine-structure constants and isotope shifts high- resolution spectroscopy on a collimated atomic beam was also employed. The behaviour of highly excited alkali atoms is mostly hydrogen- like and well predicted by theory. Group III A elements have one electron outside a closed subshell and are expected to behave like alkali atoms. The situation is however complicated by the presence of doubly excited states. Configuration interaction can then cause a partial mixing between singly and doubly excited states. In the alkaline-earth atoms (group II A elements), having two electrons outside closed shells, the situation is similar. In a Rydberg series of one excited electron the admixture of doubly excited states can cause large deviations from hydrogenic behaviour. Another complication in the alkaline-earth atoms is the mixture of singlet- and triplet states. - 4 - The presented results from measurements made on Na, Mg, Ca, Sr, Ba, Al, Ga and In will primarily serve as a basis for tests of modern atomic-physics models. Some of the lifetime values are also of astrophysical interest. Keywords: Laser spectroscopy, Rydberg states, time resolved, high resolution, two-step excitation, metastable state, two-photon absorption, frequency doubling, Raman shifting, radiative lifetime, quantum beat, hyperfine structure, isotope shift, Stark shift, alkali atoms, group III A elements, alkaline-earth atoms, configuration interaction, singlet-triplet mixing.

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Journal of Physics B Atomic Molecular and Optical Physics•May 9, 2016•49 citations
We report on the time behavior of ionization signals produced by laser excitation of Ca and Ba atomic vapor to high-Rydberg states. A space-charge-limited thermionic diode detector shows a long-lived (>I-msec) ionization signal. However, optical detection of atomic ions (Ca+, Ba+) shows that these species live for much shorter times (<100 microsec). These results, in conjunction with published results on mass-spectrometric studies of high-density atomic beams, suggest that our ionization signal is primarily due to molecular species (Ca2+, Ba2+). We also observed optically pumped amplified spontaneous emission and stimulated electronic Raman scattering in Ca+ and Ba+.
In this work radiative properties of neutral elements with one or two electrons outside closed subshells have been investigated. Using laser techniques in connection with atomic beams selective excitation of Rydberg states was performed. Most of the studied states were populated with two-step excitation. Some states were reached directly from the ground state or from a metastable state and occasionally two-photon absorption was used. The excitation sometimes involved the use of frequency-doubling and Raman- shifting techniques. By time-resolved detection of the decay light from an excited state, primarily information on the radiative lifetime is obtained. With two different experimental arrangements radiative lifetimes in several Rydberg states have been determined. Using the quantum-beat technique time-resolved detection also provides information on energy splittings. This technique was used to measure hyperfine-structure splittings.To obtain information about hyperfine-structure constants and isotope shifts high- resolution spectroscopy on a collimated atomic beam was also employed. The behaviour of highly excited alkali atoms is mostly hydrogen- like and well predicted by theory. Group III A elements have one electron outside a closed subshell and are expected to behave like alkali atoms. The situation is however complicated by the presence of doubly excited states. Configuration interaction can then cause a partial mixing between singly and doubly excited states. In the alkaline-earth atoms (group II A elements), having two electrons outside closed shells, the situation is similar. In a Rydberg series of one excited electron the admixture of doubly excited states can cause large deviations from hydrogenic behaviour. Another complication in the alkaline-earth atoms is the mixture of singlet- and triplet states. - 4 - The presented results from measurements made on Na, Mg, Ca, Sr, Ba, Al, Ga and In will primarily serve as a basis for tests of modern atomic-physics models. Some of the lifetime values are also of astrophysical interest. Keywords: Laser spectroscopy, Rydberg states, time resolved, high resolution, two-step excitation, metastable state, two-photon absorption, frequency doubling, Raman shifting, radiative lifetime, quantum beat, hyperfine structure, isotope shift, Stark shift, alkali atoms, group III A elements, alkaline-earth atoms, configuration interaction, singlet-triplet mixing.
It has been shown that a dense (>10(14) -cm(-3)) atomic vapor, irradiated by a saturating pulse of resonance radiation, will ionize on a time scale of <10(-6) sec. The ionization can be 95% complete and has been observed in Li, Na, Ca, Sr, and Ba. A large number of physical processes contribute to the ionization with different processes dominating at different stages in the ionization. These processes are discussed, and two models for calculating the ionization are described. The results of the various experiments and the applications to the spectroscopy of ions and to atomic physics studies in general are reviewed.
The method of space-charge ion detection has been extended to the case of lithium. This was accomplished by the insertion of a space-charge-limited diode into a heat-pipe oven. Lithium vapor was probed with a N2{\mathrm{N}}_{2}N2​ laser-pumped tunable dye laser from 7150 to 4400 \AA{} and with a Xe arc lamp from 7500 to 2300 \AA{}. One-through four-photon events leading to ionization were observed. The atomic transitions observed were the principal series to n=10n=10n=10 and the 2s2s2s to 3d3d3d, 4s4s4s, and 4d4d4d two-photon transitions. The two-photon absorption signals depended upon the third and fourth powers of the light intensity, indicating a new ionization process not heretofore considered important in diode signals. This new process appears to be excitation transfer from excited-state atoms to other excited-state atoms or molecules. For the high excited-state densities achieved in this experiment, this process appears to predominate over photoionization of excited-state atoms and other collisional processes involving excited-state and ground-state species. The $B\ensuremath{\leftarrow}X$, $C\ensuremath{\leftarrow}X$, and $D\ensuremath{\leftarrow}X$ molecular transitions, investigated by previous workers, were observed here.
Summary form only given. Laser-cooled atoms can be excited into Rydberg states to study Rydberg gases at high densities and low atomic velocities. Dense clouds of such atoms undergo virtually complete ionization when their density exceeds a critical value dependent on the principal quantum number n. We report a new regime in which the excited Rydberg population spontaneously evolves into long-lived high-l states, the lifetimes of which exceed the natural lifetimes of the initially excited Rydberg levels by two orders of magnitude. /sup 87/Rb atoms are collected and cooled to 50 /spl mu/K in a magneto optical trap (MOT), which is periodically turned off for 50 ms. 1 ms after the shutdown of the MOT the Rydberg atoms are created via a two-step excitation process using a 5 /spl mu/s long diode laser pulse.
Abstract In this brief review, the opportunities that the alkaline-earth elements offer for studying new aspects of Rydberg physics are discussed. For example, the bosonic alkaline-earth isotopes have zero nuclear spin which eliminates many of the complexities present in alkali Rydberg atoms, permitting simpler and more direct comparison between theory and experiment. The presence of two valence electrons allows the production of singlet and triplet Rydberg states that can exhibit a variety of attractive or repulsive interactions. The availability of weak intercombination lines is advantageous for laser cooling and for applications such as Rydberg dressing. Excitation of one electron to a Rydberg state leaves behind an optically active core ion allowing, for high- L states, the optical imaging of Rydberg atoms and their (spatial) manipulation using light scattering. The second valence electron offers the possibility of engineering long-lived doubly excited states such as planetary atoms. Recent advances in both theory and experiment are highlighted together with a number of possible directions for the future.