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Optogalvanic Measurement of Even Parity Rydberg Levels in Krypton Gas.

Kandola,M S

Published Dec 1, 1984• 0 citations
OpenAlex

Abstract

An optogalvanic detection scheme, in conjunction with a single-step pulsed laser excitation has been used to measure the energy of even parity Rydberg levels in krypton. The excitation scheme starts from the 5s(3/2)2 and 5s'(1/2)0 metastable states, which have been populated in a He-Kr discharge tube. Measured energies were compared to either calculated or previously measured values. Calculated energies were obtained with the Rydberg formula using quantum defects extrapolated from the known low-lying levels. Keywords include: Krypton, Rydberg atoms, Atomic spectra, Optogalvanic spectroscopy.

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The first detailed observation of the perturbations by an electric field of the Rydberg autoionizing resonances of a rare-gas atom is reported. The Stark spectroscopy of autoionizing Rydberg states converging to the second ionization limit $4{p}^{5}^{2}P_{\frac{1}{2}}^{o}$ in Kr I is performed in an atomic beam with the use of a two-step laser excitation from the $4{p}^{5}5s{[\frac{3}{2}]}_{2}^{0}$ metastable state. In addition to the verification of the ${({n}^{*})}^{\ensuremath{-}3}$ dependence of the zero-field width of two autoionizing series and of the linear dependence of the Stark-manifold splittings with the electric field, we have observed an ${(n)}^{0.7}$ law for the dependence of the Stark-manifold splitting along the series, an important narrowing and dissymmetrization of the $n{d}^{\ensuremath{'}}$ resonances, and a nonlinear-field behavior of Stark-manifold components in the vicinity of the first anticrossing. Discussions are carried out with the use of the recent work on Rydberg-Stark spectroscopy and on autoionizing states in two-electron atoms.

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We have implemented a new laser-based detection scheme for the rare krypton isotopes. The scheme utilizes two-step excitation of metastable krypton atoms in a nearly perfect three-level system followed by field ionization. The detection scheme was realized experimentally with a mass-separated atom beam. A total detection efficiency of about 10% is obtained.

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Two-photon spectra of Rydberg states of alkaline-earth atoms (strontium and barium)

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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
An optogalvanic detection scheme, in conjunction with a single-step pulsed laser excitation has been used to measure the energy of even parity Rydberg levels in krypton. The excitation scheme starts from the 5s(3/2)2 and 5s'(1/2)0 metastable states, which have been populated in a He-Kr discharge tube. Measured energies were compared to either calculated or previously measured values. Calculated energies were obtained with the Rydberg formula using quantum defects extrapolated from the known low-lying levels. Keywords include: Krypton, Rydberg atoms, Atomic spectra, Optogalvanic spectroscopy.
We present new experimental data on the highly excited levels in mercury using the optogalvanic detection technique in conjunction with a dc discharge cell. The collisionally populated 6s6p 3P2 metastable level has been used as an intermediate level to access the Rydberg states using a frequency-doubled dye laser covering the wavelength region between 370 and 249 nm. The optogalvanic data reveal 6sns 3S1(13≤n≤50), 6snd 2D1(6≤n≤18), 6snp 3D1(6≤n≤14), 6snd 3D2(6≤n≤15), and 6snd 3D3(6≤n≤59) Rydberg series. The 6sns 3S1 and 6snd 3D3 Rydberg series to such a high n value have been reported for the first time. In addition, collisionally induced parity-forbidden transitions 6snp 3P1(44≤n≤50) have been detected.
We have investigated a new scheme for excitation of the 5s, J = 2 metastable level of Kr (5s[3/2] J = 2 ) which can be readily extended to other rare gases. In the scheme, an ultraviolet (UV) lamp is used to create a population of Kr atoms in the 5s[3/2] J = 1 level in a gas cell. The excited atoms are then pumped to the 5p[3/2] J = 2 level, using 819 nm light from a Ti:sapphire laser, from which they decay to the metastable state with a branching ratio of 77%. We made two striking observations: (1) the laser power required to saturate the second step decreases markedly as a function of gas cell pressure, and (2) the UV photon flux is converted with very high efficiency (≈10%) to metastable atom flux. A Monte Carlo study of the scattering of UV photons in the cell reproduces the trends observed. The understanding achieved points to the design of a higher flux source of metastable atoms.
The first detailed observation of the perturbations by an electric field of the Rydberg autoionizing resonances of a rare-gas atom is reported. The Stark spectroscopy of autoionizing Rydberg states converging to the second ionization limit $4{p}^{5}^{2}P_{\frac{1}{2}}^{o}$ in Kr I is performed in an atomic beam with the use of a two-step laser excitation from the 4p55s[32]204{p}^{5}5s{[\frac{3}{2}]}_{2}^{0}4p55s[23​]20​ metastable state. In addition to the verification of the ${({n}^{*})}^{\ensuremath{-}3}$ dependence of the zero-field width of two autoionizing series and of the linear dependence of the Stark-manifold splittings with the electric field, we have observed an (n)0.7{(n)}^{0.7}(n)0.7 law for the dependence of the Stark-manifold splitting along the series, an important narrowing and dissymmetrization of the $n{d}^{\ensuremath{'}}$ resonances, and a nonlinear-field behavior of Stark-manifold components in the vicinity of the first anticrossing. Discussions are carried out with the use of the recent work on Rydberg-Stark spectroscopy and on autoionizing states in two-electron atoms.
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.