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Physical Review A

Optical pumping to the6s5dstates in atomic barium

Edmund G. Myers, C. Bell, P. G. Pappas, Daniel E. Murnick

Published Apr 1, 1986• 15 citations
Publisher

Abstract

Using a flow apparatus, the time dependence of 6${s}^{2}$ ${\mathrm{}}^{1}$${S}_{0}$--6s6p ${\mathrm{}}^{1}$${P}_{1}$ (553.5 nm) resonance fluorescence in atomic barium has been studied following switch-on of cw laser excitation. It was found that the fluorescence decays with rates as great as 1.3\ifmmode\times\else\texttimes\fi{}${10}^{6}$ ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$. Assuming this can be ascribed to the pumping of atoms to the 6s5d ${\mathrm{}}^{1}$D and $^{3}\mathrm{D}$ metastable levels, a value for the sum of the transition probabilities can be extracted.

DOI
10.1103/physreva.33.2798

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Comment on ‘‘Optical pumping to the 6s5dstates in atomic barium’’

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Frontiers of Physics•Jul 8, 2011•0 citations
Using a flow apparatus, the time dependence of 6s2{s}^{2}s2 {\mathrm{}}^{1}$${S}_{0}--6s6p {\mathrm{}}^{1}$${P}_{1} (553.5 nm) resonance fluorescence in atomic barium has been studied following switch-on of cw laser excitation. It was found that the fluorescence decays with rates as great as 1.3\ifmmode\times\else\texttimes\fi{}106{10}^{6}106 s\ensuremath−1{\mathrm{s}}^{\mathrm{\ensuremath{-}}1}s\ensuremath−1. Assuming this can be ascribed to the pumping of atoms to the 6s5d 1{\mathrm{}}^{1}1D and 3D^{3}\mathrm{D}3D metastable levels, a value for the sum of the transition probabilities can be extracted.
The resonance fluorescence from the 138Ba^{138}\mathrm{Ba}138Ba I 5535-\AA{} 6s21{\mathit{s}}^{21}s21S0{\mathit{S}}_{0}S0​-6s6p 1^{1}1P1{\mathit{P}}_{1}P1​ transition has been measured as a function of incident intensity using a Doppler-free atomic beam geometry and a single-mode cw dye laser. The upper 1P1^{1}\mathrm{P}_{1}1P1​ level has a weak branch to intermediate metastable D states. A long laser-atom interaction region was used, which ensured that essentially all atoms could be pumped into the D states during their transit through the laser beam. By analyzing the shape of the saturation curve a value for the branching ratio to the 6s5d 1^{1}1,3D levels of (3.57\ifmmode\pm\else\textpm\fi{}0.38)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}3}$ has been obtained.
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.
We describe a set of experiments that investigate diffusion of barium 6s5d3{\mathrm{}}^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​ metastable level and 6s2{\mathit{s}}^{2}s21{\mathrm{}}^{1}1S0{\mathit{S}}_{0}S0​ ground-state atoms through the noble gases: He, Ne, Ar, Kr, and Xe. The barium metastable levels were populated through optical pumping of the 6s2{\mathit{s}}^{2}s21{\mathrm{}}^{1}1S0{\mathit{S}}_{0}S0​\ensuremath{\rightarrow}6s6p3{\mathrm{}}^{3}3P1o{\mathit{P}}_{1}^{\mathit{o}}P1o​ intercombination transition with a pulsed laser, followed by spontaneous or stimulated emission into the 6s5d3{\mathrm{}}^{3}3D1,2{\mathit{D}}_{1,2}D1,2​ levels. Collisional mixing then distributed population throughout the 6s5d3{\mathrm{}}^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​ levels. A weak narrow-band cw laser was tuned to appropriate transitions to probe the spatial distribution of metastable level atoms, as well as the hole created in the ground-state spatial distribution, by the pulsed laser. Time-dependent absorption coefficients were obtained by measuring the transmission of the probe laser at several different pump-probe spatial separations. From these absorption data, spatial number density profiles were mapped out for various times following the firing of the pump laser. These density profiles were used to determine the diffusion coefficient for each state at a particular buffer-gas pressure and temperature. From these pressure- and temperature-dependent diffusion coefficients D, we determined the thermally averaged diffusion cross sections ${\mathrm{\ensuremath{\sigma}}}_{\mathit{D}}$(6s5d3{\mathrm{}}^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​) and ${\mathrm{\ensuremath{\sigma}}}_{\mathit{D}}$(6s2{\mathit{s}}^{2}s21{\mathrm{}}^{1}1S0{\mathit{S}}_{0}S0​) for the metastable and ground-state atoms diffusing through the noble gases, respectively. We also report values for the scaled standard diffusion coefficients D0{\mathit{D}}_{0}D0​. Our experimental values of the thermally averaged diffusion cross sections ${\mathrm{\ensuremath{\sigma}}}_{\mathit{D}}$(6s5d3{\mathrm{}}^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​) and ${\mathrm{\ensuremath{\sigma}}}_{\mathit{D}}$(6s2{\mathit{s}}^{2}s21{\mathrm{}}^{1}1S0{\mathit{S}}_{0}S0​) for the barium-helium system are compared with values calculated from published, theoretical barium-helium potentials and the agreement is excellent. \textcopyright{} 1996 The American Physical Society.
Rate coefficients for energy-pooling collisions between low-lying excited states of Ba have been measured. The 6s6p(3{(}^{3}(3P1{\mathit{P}}_{1}P1​) level in Ba is pumped by a cw diode laser, and radiative decay and collisions with buffer-gas atoms also populate the 5d6s(1{(}^{1}(1D) and 5d6s(3{(}^{3}(3D) metastable levels. The densities of these low-lying excited states are measured by the absorption of lines from a Ba hollow-cathode lamp, and the states populated by energy-pooling collisions are studied by comparing their fluorescence intensity to that of the laser-excited level. The rate coefficients are on the order of gas-kinetic rates, and they are not strongly dependent on energy defect, spin changes, or angular-momentum changes.
In a barium vapor pumped with laser light on the resonance transition at 553.5 nm the level 6p 1P1^{1}P_{1}1P1​ is depopulated mainly by collisional processes. With neglect of this item, radiative lifetimes derived from fluorescence measurements come out systematically too short.
Whether the transitions between 6s5d 3D and 5d6p 3F can be used for laser cooling of barium heavily depends upon the transition probabilities of 5d6p 3F-5d2 3F. Taking the transition 6s5d 3D3-5d6p 3F4 as a scale, the leakage rate of 5d6p 3F4-5d2 3F was used to evaluate the transition probabilities. 706 nm laser pulses with different durations were applied to a barium atomic beam for 6s5d 3D3-5d2 3F4 optical pumping, and the remaining percentages in 6s5d 3D3 were measured. After exponential fitting, the transition probability of 5d6p 3F4-5d2 3F3,4 was determined to be 2.1(4)×104 s−1, which is in agreement with theoretical calculations using the scaled Thomas-Fermi-Dirac method.