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Journal of Physics B Atomic and Molecular Physics

Stark mixing of high-lying calcium levels by laser-produced charges

S A Borgström, Jan R. Rubbmark

Published Dec 21, 1977• 19 citations

Abstract

Using a pulsed tunable dye laser pumped by a nitrogen laser, the 4s4p 1 P 1 0 level in Ca I was selectively populated from the 4s 2 1 S 0 ground state. Transitions from the 4s4p 1 P 1 0 level to 4sns 1 S 0 and 4snd 1 D 2 and, for n approximately=20, also to 4snp 1 P 1 0 and 4snf 1 F 3 0 were observed. The latter transitions arise because of Stark mixing of Rydberg states in the field of laser-produced ions and electrons. By applying a voltage to electrodes in the calcium vapour, Stark shifts were measured for levels belonging to the 4snf 1 F 3 0 and 4s(n+1)d 1 D 2 series in a region where the series cross. Diagonalisation of the energy matrix for interacting states with hydrogenic dipole matrix elements gave theoretical Stark shifts in reasonable agreement with those measured. The 4snf 1 F 3 0 series has been extended from n=12 to n=28 by absorption from 4s3d 1 D 2 . The latter level was found to be populated by stimulated emission from 4s4p 1 P 1 0 .

DOI: 10.1088/0022-3700/10/18/017

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Using a pulsed tunable dye laser pumped by a nitrogen laser, the 4s4p 1 P 1 0 level in Ca I was selectively populated from the 4s 2 1 S 0 ground state. Transitions from the 4s4p 1 P 1 0 level to 4sns 1 S 0 and 4snd 1 D 2 and, for n approximately=20, also to 4snp 1 P 1 0 and 4snf 1 F 3 0 were observed. The latter transitions arise because of Stark mixing of Rydberg states in the field of laser-produced ions and electrons. By applying a voltage to electrodes in the calcium vapour, Stark shifts were measured for levels belonging to the 4snf 1 F 3 0 and 4s(n+1)d 1 D 2 series in a region where the series cross. Diagonalisation of the energy matrix for interacting states with hydrogenic dipole matrix elements gave theoretical Stark shifts in reasonable agreement with those measured. The 4snf 1 F 3 0 series has been extended from n=12 to n=28 by absorption from 4s3d 1 D 2 . The latter level was found to be populated by stimulated emission from 4s4p 1 P 1 0 .

The Stark shift of the (4s

{)}^{2}

{\mathrm{}}^{1}

{\mathit{S}}_{0}

\ensuremath{\rightarrow}(4s4p)

{\mathrm{}}^{3}

{\mathit{P}}_{1}

transition in calcium was measured using a laser to excite an atomic beam as it traversed through a uniform electric field and a field-free region. The laser frequency was scanned across the transition, while fluorescence produced by the radiative decay of the excited state was detected. The frequency scan was calibrated using an acousto-optic modulator to frequency shift part of the laser beam. The Stark shift rate was found to be -12.314\ifmmode\pm\else\textpm\fi{}0.041 kHz/(kV/cm

{)}^{2}

, where the minus sign indicates the transition frequency decreases when the electric field is applied. \textcopyright{} 1996 The American Physical Society.

Calcium Rydberg levels are of significant interest for efficient and isotope-selective resonance ionization of trace radionuclides such as calcium-41 ( 41 Ca). In this study, we report novel, to our knowledge, measurement data on the energy level shifts of 43 Ca for 4sns 1 S 0 and 4s(n−1)d 1 D 2 (n=40, 45, 50, 55, 60) Rydberg levels due to hyperfine-induced singlet–triplet mixing specific to isotopes with an odd mass number. Both 3 S 1 and 3 D J triplet signals corresponding to forbidden transitions were enhanced for 43 Ca at the high principal quantum numbers n=55 and 60, indicating a mixing of singlet components to some extent.

Experiments on collisionally assisted two-photon absorption (TPA) in calcium vapour buffered by argon gas have been performed using two tunable dye lasers. Both direct TPA and stepwise transitions through the collisionally populated resonance level. 4s4p 1 P 1 , have been observed. Detailed study of the lineshapes of the stepwise transitions to the 4p 2 1 S 0 , 4p 2 1 D 2 and 4s6s 1 S 0 levels reveals large differences in the strengths of the Ca-Ar interatomic potentials for these levels. These differences probably arise from configuration mixing.

An experiment is described in which large numbers ( approximately 10 16 ) of calcium atoms are placed in the 4s4p 3 P metastable level by optical pumping with a tunable dye laser and then studied spectroscopically. Equations governing the degree of excitation by the laser are derived. Predictions of the theory are shown to be in good agreement with experimental results. In particular, at low optical depths produced by 10 15 ground state atoms cm -2 the dye laser raises approximately 50% of the calcium atoms into the metastable state. At higher optical depths associated with 10 17 ground state atoms cm -2 the number of excited states is limited only by the laser energy and line width. For the dye laser used the largest number of metastables produced was approximately 10 16 . The absorption spectra of the 4s4p 2 P level is seen out to 4s4p 3 P to 4s22d 3 D. The relaxation rate between the excited state fine structure is studied directly with an optically delayed dye laser continuum. Other applications of this technique of producing large numbers of excited states are briefly discussed.

Experimental results on the ionization of calcium atoms following resonant pumping of the 4s 2 1 S 0 -4s4p 3 P 1 transition with a CW ring dye laser are reported. Absorption profiles of the 4s 2 1 S 0 -4s4p 3 P 1 transition around 6572.78 AA are measured under different conditions of temperature (T) and buffer gas pressure (p) where ionization was observed. Voigt profile fits are seen to adequately describe the observed absorption profiles. The results on collisional widths are in agreement with some previously published measurements. At low buffer gas pressures, collisional widths are found to scale as T 0.5 .