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Journal of Physics B Atomic Molecular and Optical Physics

Collisional shifts and broadenings of doubly excited states of barium

M. Marafi, Z Suji, K. S. Bhatia, Joseph Mathew

Published Oct 1, 2008• 7 citations
Publisher

Abstract

Shift and broadening parameters for doubly excited states of 5d6d, 5d7d, 5d7s, 5d8s and 6p 2 configurations in neutral barium atoms are presented. A tunable dye laser pumped by an excimer laser was used to populate the Rydberg states of Ba by two-photon absorption from the 6s 2 1 S 0 ground state. Inert gases Ar, Kr and Xe at 100 mbar pressure were used as perturbing gases. The resulting line shapes were fitted to a Voigt line shape function, from which shift and broadening parameters were inferred.

DOI
10.1088/0953-4075/41/20/205203

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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.

•Jan 1, 2008•0 citations
Shift and broadening parameters for doubly excited states of 5d6d, 5d7d, 5d7s, 5d8s and 6p 2 configurations in neutral barium atoms are presented. A tunable dye laser pumped by an excimer laser was used to populate the Rydberg states of Ba by two-photon absorption from the 6s 2 1 S 0 ground state. Inert gases Ar, Kr and Xe at 100 mbar pressure were used as perturbing gases. The resulting line shapes were fitted to a Voigt line shape function, from which shift and broadening parameters were inferred.
Collisional broadening and shift data for even parity states of neutral barium are presented. A two-photon absorption technique is used to populate Rydberg states of n d 1 D 2 , 3 D 2 and 1 S 0 series. High-resolution Ba excitation spectra were measured using a diode detector while scanning the frequency of an excimer pumped dye laser. Inert gases Ar, Kr and Xe were used as perturbers at pressures ranging from 10 mb to 400 mb. Shifts and broadenings of spectral lines were measured as a function of pressure and principal quantum number n . Several perturbations and deviations from expected results are discussed in this paper.
Energy-pooling collisions between low-lying excited states of Ba have been studied. We have used a CW dye laser to excite the level in Ba. Radiative decay and collisions with Ba or buffer-gas atoms (Ar, He) populate also the , and metastable levels. The spatial density distributions of these excited levels were measured by the absorption of lines from a Ba hollow-cathode lamp as a function of laser frequency. When the laser was on the exact atomic resonance we observed fluorescence from the , , , , , , and states populated by energy-pooling collisions of Ba( , ). By changing the buffer gas pressure the fluorescence intensity ratio between - and - transitions changes dramatically. This is found to be due to redistribution of population among metastable levels, both in magnitude and space. In addition, we have found that the and metastable levels are also populated when the laser is tuned to the blue from the 553.5 nm line under which conditions a pronounced red-shifted light cone (cone emission) is observed.
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.