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Optics Letters

Enhancement of Rb fine-structure transfer in ^4He due to three-body collisions

J. F. Sell, M. A. Gearba, Brian M. Patterson, T. Genda, B. Naumann, R. J. Knize

Published Jun 16, 2010• 10 citations
Publisher

Abstract

Using ultrafast laser excitation and time-correlated single-photon counting techniques, we have measured the collisional mixing rates between the rubidium 5(2)P fine-structure levels in the presence of (4)He gas. A nonlinear dependence of the mixing rate with (4)He density is observed. We find Rb fine-structure transfer is primarily due to binary collisions at (4)He densities of < or = 10(19) cm(-3), while at greater densities, three-body collisions become significant. We determine a three-body collisional transfer rate coefficient (5(2)P(3/2) --> 5(2)P(1/2)) of 1.25(9)x10(-32) cm(6)/s at 22 degrees C.

DOI
10.1364/ol.35.002146

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Using ultrafast laser excitation and time-correlated single-photon counting techniques, we have measured the collisional mixing rates between the rubidium 5(2)P fine-structure levels in the presence of (4)He gas. A nonlinear dependence of the mixing rate with (4)He density is observed. We find Rb fine-structure transfer is primarily due to binary collisions at (4)He densities of < or = 10(19) cm(-3), while at greater densities, three-body collisions become significant. We determine a three-body collisional transfer rate coefficient (5(2)P(3/2) --> 5(2)P(1/2)) of 1.25(9)x10(-32) cm(6)/s at 22 degrees C.
Employing ultrafast laser excitation and time-correlated single-photon counting, we have measured the fine-structure transfer between Rb 5P states induced by collisions with 4He buffer gas at temperatures up to 150 °C. The temperature dependence of the binary cross section agrees with earlier measurements. Our data show that the temperature dependence of the three-body rate is about the same as that of the binary rate. The three-body rate can be described as arising from the reduction of the rubidium fine-structure splitting due to nearby helium atoms.
Measurements of the mixing rates and cross sections for collisional excitation transfer between the 5P 1/2 and 5P 3/2 states of rubidium (Rb) in the presence of 4 He buffer gas are presented. Selected pulses from a high repetition rate, mode-locked femtosecond laser are used to excite either Rb state with the fluorescence due to collisional excitation transfer observed by time-correlated single-photon counting. The time dependence of this fluorescence is fitted to the solution of rate equations which include the mixing rate, atomic lifetimes and any quenching processes. The variation in the mixing rate over a large range of buffer gas densities allows the determination of both the binary collisional transfer cross section and a three-body collisional transfer rate. We do not observe any collisional quenching effects at 4 He pressures up to 6 atm and discuss in detail other systematic effects considered in the experiment.
We have examined fine-structure mixing between the rubidium 52P3/25\phantom{\rule{0.16em}{0ex}}^{2}P_{3/2}52P3/2​ and 52P1/25\phantom{\rule{0.16em}{0ex}}^{2}P_{1/2}52P1/2​ states along with quenching of these states due to collisions with methane gas. Measurements are carried out using ultrafast laser-pulse excitation to populate one of the Rb 52P5{\phantom{\rule{0.16em}{0ex}}}^{2}P52P states, with the fluorescence produced through collisional excitation transfer observed using time-correlated single-photon counting. Fine-structure mixing rates and quenching rates are determined by the time dependence of this fluorescence. As Rb(52P\mathrm{Rb}(5\phantom{\rule{0.16em}{0ex}}^{2}PRb(52P) collisional excitation transfer is relatively fast in methane gas, measurements were performed at methane pressures of 2.5−−252.5--252.5−−25 Torr, resulting in a collisional transfer cross section ($5\phantom{\rule{0.16em}{0ex}}^{2}P_{3/2}\ensuremath{\rightarrow}5\phantom{\rule{0.16em}{0ex}}^{2}P_{1/2}$) of $(4.23\ifmmode\pm\else\textpm\fi{}0.13)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}15}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{2}$. Quenching rates were found to be much slower and were performed over methane pressures of 50−−400050--400050−−4000 Torr, resulting in a quenching cross section of $(7.52\ifmmode\pm\else\textpm\fi{}0.10)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}19}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{2}$. These results represent a significant increase in precision compared to previous work, and also resolve a discrepancy in previous quenching measurements.
Rb atoms were excited to the 5P3/2 level using a single-mode laser diode. The 5P3/2 state atom density was measured by the absorption of line from a Rb hollow-cathode lamp. The excited atom density is combined with measured fluorescence ratio to determine collisional cross section for the energy pooling process [i.e. Rb(5P3/2)+Rb(5P3/2)→Rb(5D)+Rb(5S)]. The cross section is (5.0±1.9)(?)10-14cm2. Cross section for 5P3/2 →5P1/2 transfer in Rb, induced in collision with ground-state Rb atoms, has been determined using methods of atomic fluorescence. The resulting fluorescence included a direct component arising from the optically excited state and a sensitized component due to the collisionally populated fine-structure state and the energy-pooling collisions. Measurement of relative intensities of the two components yielded the following cross section: σ(5P3/2→5P1/2)=(3.0±0.9)×10-15cm2. It is found that the rate for the energy pooling is an order of magnitude more efficient than 5P3/2→5P1/2 mixture. Comparisons of our result with other experiments have been made.
Inelastic collisional processes in fine-structure-state mixing have been studied by selective stepwise excitation and observation of the resulting fluorescence during collisions of excited rubidium 62D526^{2}D_{\frac{5}{2}}62D25​​ state atoms with various noble-gas atoms. It is shown that for intermediately excited rubidium atoms the fine-structure-state mixing cross sections are generally increasing from helium to xexon. The cross sections for the process $\mathrm{Rb}(6^{2}D_{\frac{5}{2}})+A(n^{1}S_{0})\ensuremath{\rightarrow}\mathrm{Rb}(6^{2}D_{\frac{3}{2}})+A(n^{1}S_{0})+\ensuremath{\Delta}E$ have the values ${\ensuremath{\sigma}}_{\mathrm{fs}}^{*}=2.4\ifmmode\pm\else\textpm\fi{}0.9, 3.1\ifmmode\pm\else\textpm\fi{}1.2, 2.6\ifmmode\pm\else\textpm\fi{}1.0, 5.8\ifmmode\pm\else\textpm\fi{}2.2, \mathrm{and} 9.3\ifmmode\pm\else\textpm\fi{}5.6$ in units of ${10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2, where AAA denotes in sequence any one of the noble gas atoms He, Ne, Ar, Kr, and Xe, respectively. Transfer cross sections for the transfer of excited Rb62D6^{2}D62D-state atoms out of the doublet were also determined and are about an order of magnitude smaller than the fine-structure-mixing cross sections.
We report a study of fine-structure mixing $\mathrm{Rb}(5{}^{2}{D}_{5/2})\ensuremath{\rightarrow}\mathrm{Rb}(5{}^{2}{D}_{3/2})$ in collisions with ground-state Rb atoms. In the experiment, two-photon cw laser excitation was applied to the Rb vapor cell. The measured cross section for the process was $(5.8\ifmmode\pm\else\textpm\fi{}1.9)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}{\mathrm{cm}}^{2}.$ Theoretical calculations using nonadiabatic collision theory gave a value of $3.4\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}{\mathrm{cm}}^{2}.$