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Physical Review A

Hyperfine state-changing collisions of Cs(6P1∕2) atoms with argon perturbers

L. Morgus, T. Morgus, Tyler Drake, John Huennekens

Published Mar 10, 2008• 3 citations
Publisher

Abstract

A two-step excitation experiment has been employed to measure the collisional rate coefficients and to study the velocity distribution of $\mathrm{Cs}(6{P}_{1∕2})$ atoms that have undergone a single hyperfine state-changing collision with Ar. In addition, argon pressure broadening rates and shifts of the cesium $6{P}_{1∕2}({F}^{\ensuremath{'}})\ensuremath{\rightarrow}8{S}_{1∕2}({F}^{\ensuremath{''}})$ transitions have been determined. In the experiment, a single mode, cw Ti:sapphire laser is tuned to line center of the $6{S}_{1∕2}(F=4)\ensuremath{\rightarrow}6{P}_{1∕2}$(${F}^{\ensuremath{'}}=3$ or 4) transition. Then, the frequency of a single mode cw dye laser is scanned over the $6{P}_{1∕2}\ensuremath{\rightarrow}8{S}_{1∕2}$ manifold to probe the populations of the $6{P}_{1∕2}$ hyperfine levels. Absorption of probe laser photons is monitored by detecting $8{S}_{1∕2}\ensuremath{\rightarrow}6{P}_{3∕2}$ fluorescence. The experiment is conducted at room temperature, where the Cs density is low $(n\ensuremath{\sim}3.4\ifmmode\times\else\texttimes\fi{}{10}^{10}\phantom{\rule{0.3em}{0ex}}\mathrm{atoms}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3})$, and thus the probability of a $\mathrm{Cs}\text{\ensuremath{-}}\mathrm{Cs}$ collision is negligible during the $\mathrm{Cs}(6{P}_{1∕2})$ radiative lifetime. The Ar pressure is varied from 0 to $1.52\phantom{\rule{0.3em}{0ex}}\mathrm{Torr}$, and $\mathrm{Cs}\text{\ensuremath{-}}\mathrm{Ar}$ collisions cause population to be transferred from the directly excited $6{P}_{1∕2}({F}^{\ensuremath{'}})$ level to the other $6{P}_{1∕2}$ hyperfine level. The data are analyzed using a density matrix formalism to yield the rate coefficients for $\mathrm{Cs}(6{P}_{1∕2})\text{\ensuremath{-}}\mathrm{Ar}$ hyperfine state-changing collisions. In addition, the one-dimensional velocity changing collision kernel for $\mathrm{Cs}(6{P}_{1∕2})$ atoms prepared with ${v}_{z}=0$ that undergo ${F}^{\ensuremath{'}}=3\ensuremath{\leftrightarrow}{F}^{\ensuremath{'}}=4$ hyperfine state-changing collisions with argon is reported.

DOI
10.1103/physreva.77.032704

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Physical Review A•Aug 1, 1996•41 citations
A two-step excitation experiment has been employed to measure the collisional rate coefficients and to study the velocity distribution of Cs(6P1∕2)\mathrm{Cs}(6{P}_{1∕2})Cs(6P1∕2​) atoms that have undergone a single hyperfine state-changing collision with Ar. In addition, argon pressure broadening rates and shifts of the cesium 6P1∕2(F\ensuremath′)\ensuremath→8S1∕2(F\ensuremath′′)6{P}_{1∕2}({F}^{\ensuremath{'}})\ensuremath{\rightarrow}8{S}_{1∕2}({F}^{\ensuremath{''}})6P1∕2​(F\ensuremath′)\ensuremath→8S1∕2​(F\ensuremath′′) transitions have been determined. In the experiment, a single mode, cw Ti:sapphire laser is tuned to line center of the 6S1∕2(F=4)\ensuremath→6P1∕26{S}_{1∕2}(F=4)\ensuremath{\rightarrow}6{P}_{1∕2}6S1∕2​(F=4)\ensuremath→6P1∕2​(F\ensuremath′=3{F}^{\ensuremath{'}}=3F\ensuremath′=3 or 4) transition. Then, the frequency of a single mode cw dye laser is scanned over the 6P1∕2\ensuremath→8S1∕26{P}_{1∕2}\ensuremath{\rightarrow}8{S}_{1∕2}6P1∕2​\ensuremath→8S1∕2​ manifold to probe the populations of the 6P1∕26{P}_{1∕2}6P1∕2​ hyperfine levels. Absorption of probe laser photons is monitored by detecting 8S1∕2\ensuremath→6P3∕28{S}_{1∕2}\ensuremath{\rightarrow}6{P}_{3∕2}8S1∕2​\ensuremath→6P3∕2​ fluorescence. The experiment is conducted at room temperature, where the Cs density is low (n\ensuremath∼3.4\ifmmode×\else\texttimes\fi1010atomscm\ensuremath−3)(n\ensuremath{\sim}3.4\ifmmode\times\else\texttimes\fi{}{10}^{10}\phantom{\rule{0.3em}{0ex}}\mathrm{atoms}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3})(n\ensuremath∼3.4\ifmmode×\else\texttimes\fi1010atomscm\ensuremath−3), and thus the probability of a Cs\ensuremath-Cs\mathrm{Cs}\text{\ensuremath{-}}\mathrm{Cs}Cs\ensuremath-Cs collision is negligible during the Cs(6P1∕2)\mathrm{Cs}(6{P}_{1∕2})Cs(6P1∕2​) radiative lifetime. The Ar pressure is varied from 0 to 1.52Torr1.52\phantom{\rule{0.3em}{0ex}}\mathrm{Torr}1.52Torr, and Cs\ensuremath-Ar\mathrm{Cs}\text{\ensuremath{-}}\mathrm{Ar}Cs\ensuremath-Ar collisions cause population to be transferred from the directly excited 6P1∕2(F\ensuremath′)6{P}_{1∕2}({F}^{\ensuremath{'}})6P1∕2​(F\ensuremath′) level to the other 6P1∕26{P}_{1∕2}6P1∕2​ hyperfine level. The data are analyzed using a density matrix formalism to yield the rate coefficients for Cs(6P1∕2)\ensuremath-Ar\mathrm{Cs}(6{P}_{1∕2})\text{\ensuremath{-}}\mathrm{Ar}Cs(6P1∕2​)\ensuremath-Ar hyperfine state-changing collisions. In addition, the one-dimensional velocity changing collision kernel for Cs(6P1∕2)\mathrm{Cs}(6{P}_{1∕2})Cs(6P1∕2​) atoms prepared with vz=0{v}_{z}=0vz​=0 that undergo F\ensuremath′=3\ensuremath↔F\ensuremath′=4{F}^{\ensuremath{'}}=3\ensuremath{\leftrightarrow}{F}^{\ensuremath{'}}=4F\ensuremath′=3\ensuremath↔F\ensuremath′=4 hyperfine state-changing collisions with argon is reported.
We report experimental rate coefficients for the energy-pooling collisions Cs(6P1/2{\mathit{P}}_{1/2}P1/2​)+Cs(6P1/2{\mathit{P}}_{1/2}P1/2​)\ensuremath{\rightarrow}Cs(6S1/2{\mathit{S}}_{1/2}S1/2​)+Cs(${\mathit{nl}}_{\mathit{J}\ensuremath{'}}$) and Cs(6P3/2{\mathit{P}}_{3/2}P3/2​)+Cs(6P3/2{\mathit{P}}_{3/2}P3/2​)\ensuremath{\rightarrow}Cs(6S1/2{\mathit{S}}_{1/2}S1/2​)+Cs(${\mathit{nl}}_{\mathit{J}\ensuremath{'}}$) where ${\mathit{nl}}_{\mathit{J}\ensuremath{'}}$=7P1/2{\mathit{P}}_{1/2}P1/2​, 7P3/2{\mathit{P}}_{3/2}P3/2​, 6D3/2{\mathit{D}}_{3/2}D3/2​, 6D5/2{\mathit{D}}_{5/2}D5/2​, 8S1/2{\mathit{S}}_{1/2}S1/2​, 4F5/2{\mathit{F}}_{5/2}F5/2​, or 4F7/2{\mathit{F}}_{7/2}F7/2​. Atoms were excited to either the 6P1/2{\mathit{P}}_{1/2}P1/2​ or 6P3/2{\mathit{P}}_{3/2}P3/2​ state using a single-mode Ti:sapphire laser. The excited-atom density and spatial distribution were mapped by monitoring the absorption of a counterpropagating single-mode ring dye laser beam, tuned to either the 6P1/2{\mathit{P}}_{1/2}P1/2​\ensuremath{\rightarrow}8S1/2{\mathit{S}}_{1/2}S1/2​ or 6P3/2{\mathit{P}}_{3/2}P3/2​\ensuremath{\rightarrow}7D3/2,5/2{\mathit{D}}_{3/2,5/2}D3/2,5/2​ transitions, which could be translated parallel to the pump beam. Transmission factors, which describe the average probability that photons emitted within the fluorescence detection region can pass through the optically thick vapor without being absorbed, were calculated for all relevant transitions. Effective lifetimes of levels populated by energy-pooling collisions are modified by radiation trapping, and these factors were calculated using the Molisch theory. These calculated quantities have been combined with the measured excited-atom densities and fluorescence ratios to yield absolute energy-pooling rate coefficients. It was found that the rate for production, in all cases, is greatest for 6D, but that 1/2-1/2 collisions are significantly more efficient than 3/2-3/2 collisions for populating 7P. It was also found that 7P1/2{\mathit{P}}_{1/2}P1/2​ is populated two to three times more efficiently than 7P3/2{\mathit{P}}_{3/2}P3/2​ in 1/2-1/2 collisions, but that the 7P fine-structure levels are approximately equally populated in 3/2-3/2 collisions. \textcopyright{} 1996 The American Physical Society.
The effective radiative rate for Cs(6P3/2) resonance level in the presence of Ar is determined.Cs atoms were excited to the 6P3/2 state using a single-mode diode laser(pump laser).The excited-atom density and spatial distribution were mapped by monitoring the absorption of a counterpropagating single-mode diode laser beam(probe laser),tuned to the 6P3/28S1/2 transition which could be translated parallel to the pump beam.In the presence of radiation trapping,the spontaneous radiation rate is multiplied by the transmission factor T6p3/26S1/2,which describes the average probability that photons emitted within the fluorescence detection region can pass through the optically thick vapor without being absorbed.Position dependent 6P3/2 state densities had been combined with the collisional broadening rate 6P3/26S1/2 line due to both Ar and cesium perturbers to yield the T6p3/26S1/2.The effective radiative rates of the Cs D2 line as a function of the Ar pressure PAr were obtained.The fluorescence intensity I852 of the 6P3/26S1/2emission was measured simultaneously.The measured fluorescence ratios determined the ratios of the effective radiative rates at different Ar density.These ratios are in agreement with theoretical evaluation.
The excited state population distribution created by 6S1/2 --> 6P3/2 laser excitation in room temperature cesium vapor mixed with Ar was quantitatively analyzed applying absorption and saturation spectroscopy. A simple method for the determination of the excited state population in a single excitation step based on the measurements of the saturated and unsaturated absorption coefficients was tested. When the line profile is nearly pure Doppler and the laser linewidth is much smaller than the inhomogeneous linewidth but comparable with homogeneous linewidth, the fraction N(v(z)) of the atoms in the ground state that are able to absorb under inhomogeneous broadening conditions can be determined. The transmission of the medium in the center of the Doppler envelope of the strong h. f. component of the CsD2 line due to hyperfine pumping alone amounts to approximately 5%. The assumption that has been made is that the lower-state hyperfine levels are populated in a statistical ratio. The absorption coefficients were measured for a series of P852 powers between 20 microW and 2. 5 mW. The velocity selective population density in the 6P3/2 state was obtained. The population in the 6P3/2 level obtained from the saturation measurements was also determined by the absorption measurement of narrow spectral line from a Cs hollow cathode lamp. The agreement between the results obtained in these two ways is very good. It was shown that 5% of the ground state population could be transferred to the first excited state by pumping the Doppler broadened line with a single-mode narrow-band laser. The argon caused line broadening and therefore increased the effective pumping rate in the first excitation step. The dependence of the 852 nm line fluorescence intensity was plotted against the population in the 6P3/2 level determined from the saturation absorption. This can serve as confirmation of the reliability of the method used for the determination of the excited state population.
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We report an experimental investigation of the excitation-transfer collision Cs(5D5/2{D}_{5/2}D5/2​)+Cs(6S)\ensuremath{\rightarrow}CS ((5D3/2{D}_{3/2}D3/2​)+Cs(6S). The upper 5D5/2{D}_{5/2}D5/2​ state was excited by a cw dye laser tuned to the one-photon, quadrupole-allowed 6S\ensuremath{\rightarrow}5D5/2{D}_{5/2}D5/2​ transition. Since the direct 5D\ensuremath{\rightarrow}6P fluorescence could not be detected with our apparatus, we monitored instead the cascade 6P\ensuremath{\rightarrow}6S fluorescence. The ratio of 6P1/2{P}_{1/2}P1/2​ to 6P3/2{P}_{3/2}P3/2​ fluorescence contains information on the collisional mixing that takes place in the 5D levels but also includes a significant contribution from mixing in the 6P levels. This latter contribution could effectively be subtracted out using the results of a second experiment in which a tunable cw diode laser was used to pump the 6P3/2{P}_{3/2}P3/2​ state, and the same fluorescence ratio monitored. The 5D mixing cross section we obtain, 70 A˚2{\r{}}^{2}˚2, is significantly larger than previous indirect determinations.
We report experimental rate coefficients for the energy-pooling collisions Cs(6{ital P}{sub 1/2})+Cs(6{ital P}{sub 1/2}){r_arrow}Cs(6{ital S}{sub 1/2})+Cs({ital nl}{sub {ital J}{prime}}) and Cs(6{ital P}{sub 3/2})+Cs(6{ital P}{sub 3/2}){r_arrow}Cs(6{ital S}{sub 1/2})+Cs({ital nl}{sub {ital J}{prime}}) where {ital nl}{sub {ital J}{prime}}=7{ital P}{sub 1/2}, 7{ital P}{sub 3/2}, 6{ital D}{sub 3/2}, 6{ital D}{sub 5/2}, 8{ital S}{sub 1/2}, 4{ital F}{sub 5/2}, or 4{ital F}{sub 7/2}. Atoms were excited to either the 6{ital P}{sub 1/2} or 6{ital P}{sub 3/2} state using a single-mode Ti:sapphire laser. The excited-atom density and spatial distribution were mapped by monitoring the absorption of a counterpropagating single-mode ring dye laser beam, tuned to either the 6{ital P}{sub 1/2}{r_arrow}8{ital S}{sub 1/2} or 6{ital P}{sub 3/2}{r_arrow}7{ital D}{sub 3/2,5/2} transitions, which could be translated parallel to the pump beam. Transmission factors, which describe the average probability that photons emitted within the fluorescence detection region can pass through the optically thick vapor without being absorbed, were calculated for all relevant transitions. Effective lifetimes of levels populated by energy-pooling collisions are modified by radiation trapping, and these factors were calculated using the Molisch theory. These calculated quantities have been combined with the measured excited-atom densities and fluorescence ratios to yield absolute energy-pooling rate coefficients. It was found that the rate formore » production, in all cases, is greatest for 6{ital D}, but that 1/2-1/2 collisions are significantly more efficient than 3/2-3/2 collisions for populating 7{ital P}. It was also found that 7{ital P}{sub 1/2} is populated two to three times more efficiently than 7{ital P}{sub 3/2} in 1/2-1/2 collisions, but that the 7{ital P} fine-structure levels are approximately equally populated in 3/2-3/2 collisions. {copyright} {ital 1996 The American Physical Society.}« less