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Journal of Physics B Atomic and Molecular Physics

Optical-optical double resonance in barium

Jörg Neukammer, Herbert H. Rinneberg

Published Sep 4, 1982• 12 citations
Publisher

Abstract

Using two CW dye lasers barium Rydberg states were populated by stepwise two-photon absorption via the 6s6p 1 P 1 intermediate level. Monitoring the transmission of the first laser beam, tuned to the resonance line, and scanning the second laser across the upper atomic transition, a greatly enhanced signal was observed. Taking optical pumping into account, a simple rate equation model can quantitatively describe the increase in sensitivity. This technique was applied to measure the hyperfine structure of the 6s15d 1 D 2 Rydberg state in barium.

DOI
10.1088/0022-3700/15/17/022

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We apply two-photon resonant nondegenerate four-wave mixing with a resonant intermediate state to the observation of the broadening and shifting of the barium Rydberg level 6s24d 1D2 by collision with argon.The collision broadening and shifting cross sections are measured.This technique is purely optical,and can investigate the pressure dependence of the transverse relaxation rate Γ21 between the Rydberg state and an intermediate state,as well as the transverse relaxation rate Γ20 between the Rydberg state and the ground state.

中国物理B：英文版•Jan 1, 2012•0 citations
Using two CW dye lasers barium Rydberg states were populated by stepwise two-photon absorption via the 6s6p 1 P 1 intermediate level. Monitoring the transmission of the first laser beam, tuned to the resonance line, and scanning the second laser across the upper atomic transition, a greatly enhanced signal was observed. Taking optical pumping into account, a simple rate equation model can quantitatively describe the increase in sensitivity. This technique was applied to measure the hyperfine structure of the 6s15d 1 D 2 Rydberg state in barium.
The Stark shift of the (6s)2{)}^{2})2 1^{1}1S0{\mathit{S}}_{0}S0​\ensuremath{\rightarrow}(6s6p)1{)}^{1})1P1{\mathit{P}}_{1}P1​ transition in barium was measured using a laser to excite an atomic beam as it traversed 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 which frequency shifted the laser by a specified amount. The Stark-shift rate was found to be -28.532\ifmmode\pm\else\textpm\fi{}0.060 kHz/(kV/cm)2{)}^{2})2. The hyperfine splitting of the 135,137Ba^{135,137}\mathrm{Ba}135,137Ba F=1/2 level relative to 138Ba^{138}\mathrm{Ba}138Ba of the (6s6p)1{)}^{1})1P1{\mathit{P}}_{1}P1​ state was determined to be -549.47\ifmmode\pm\else\textpm\fi{}0.12 MHz, where the minus sign indicates that the 138Ba^{138}\mathrm{Ba}138Ba transition is at a lower frequency.
An ongoing spectroscopic investigation of atomic rubidium utilizes a two-photon, single-laser excitation process. Transitions accessible with our tunable laser include 5P1/2 (F ′ ) ← 5S1/2 (F) and 5P3/2 (F ′ ) ← 5S1/2 (F). The laser is split into a pump and probe beam to allow for Doppler-free measurements of transitions between hyperfine levels. The pump and probe beams are overlapped in a counter-propagating geometry and the laser frequency scans over a transition. Absorption, fluorescence and polarization spectroscopy techniques are applied to this basic experimental setup. The temperature of the vapor cell and the power of the pump and probe beams have been varied to explore line broadening effects and signal-to-noise of each technique. This humble setup will hopefully grow into a more robust experimental arrangement in which double resonance, two-laser excitations are used to explore hyperfine state changing collisions between rubidium atoms and noble gas atoms. Rb-noble gas collisions can transfer population between hyperfine levels, such as 5P3/2 (F ′ = 3) Collision ←− 5P3/2 (F ′ = 2), and the probe beam couples 7S1/2 (F ′′ = 2) ← 5P3/2 (F ′ = 3). Polarization spectroscopy signal depends on the rate of population transfer due to the collision as well as maintaining the orientation created by the pump laser. Fluorescence spectroscopy relies only on transfer of population due to the collision. Comparison of these techniques yields information regarding the change of the magnetic sublevels, mF , during hyperfine state changing collisions.
We have observed kilohertz and sub-kilohertz resonance structures in RF-optical double resonance experiments of rare-earth-doped solids, when the frequency of the RF field is scanned across the hyperfine transitions while monitoring the resonant optical absorption of a CW laser. The effect is observed only when the laser spectral width is broad compared to the hyperfine structure. The observed line widths are apparently free of the inhomogeneous widths of hyperfine levels and the line shape has peculiar double peak structure. The effect is modelled with a resonance involving three atomic levels interacting with three electromagnetic fields, two optical and one RF, in a triangular or “delta’ configuration. While the ordinary optical-RF two-field resonance is limited by spin inhomogeneous width, the simultaneous excitation of three coupled transitions leads to narrow and highly nonlinear resonance structures that are not averaged by the inhomogeneous distribution of hyperfine transition.
This is the first reported demonstration of the use of pair-absorption transitions for optically pumping lasers. In a mixture of barium and thallium metal vapors, single-photon absorption of 3867-A laser light caused simultaneous excitation of colliding ground-state atoms to the Ba(6s6p 1P1(o)) and Tl(6p 2P(3/2)(o)) excited states. Excited-state densities of about 10(14) cm(-3) were created, and subsequent laser emission on the Ba(6s6p 1PI(o)) - Ba(6s5d 1D2) atomic transition at 1.5 microm was observed.
Odd-parity barium Rydberg states have been populated by stepwise excitation via M1-E1 and E2-E1 transitions, starting from the 6s2 1S0 ground state. Using two cw dye ring lasers and employing thermionic detection, Doppler-free spectra of 6snp 1,3P and 6snf 1,3F Rydberg states have been recorded with excellent signal/noise ratios. A systematic study of the hyperfine structure of 6snp 1P1 Rydberg states has been carried out. Between n=20 and n=23 a resonance in singlet-triplet mixing occurs caused by configuration interaction with the 5d8p 1P1 perturbing state, located close to the first ionization limit. Our results are in disagreement with an existing multichannel quantum defect analysis of this series. The singlet-triplet mixing of 6snp 1P1 and 6snd 1D2 Rydberg series is compared.
We apply two-photon resonant nondegenerate four-wave mixing with a resonant intermediate state to the observation of the broadening and shifting of the barium Rydberg level 6s24d 1D2 by collision with argon.The collision broadening and shifting cross sections are measured.This technique is purely optical,and can investigate the pressure dependence of the transverse relaxation rate Γ21 between the Rydberg state and an intermediate state,as well as the transverse relaxation rate Γ20 between the Rydberg state and the ground state.