Abstract The rates for fine structure mixing and quenching of the moderately excited 8 2 D 5 / 2 and 8 2 D 3 / 2 states of cesium under collision with argon and the more impulsive helium have been measured, using two-photon pulsed excitation and time-resolved fluorescence techniques. The pressure dependence of the eigenvalues of the rate matrix yields very rapid rate coefficients of 2.6 ± 0.2 × 10 − 9 cm 3 / ( atom s ) for He and 5.2 ± 0.4 × 10 − 10 cm 3 / ( atom s ) for Ar, about two–three times faster than for the Cs 7 2 D 5 / 2 ⇌ 7 2 D 3 / 2 relaxation. The quenching rates are also rapid, 1.07 ± 0.04 × 10 − 10 cm 3 / ( atom s
Abstract The rates for fine structure mixing and quenching of the moderately excited 8 2 D 5 / 2 and 8 2 D 3 / 2 states of cesium under collision with argon and the more impulsive helium have been measured, using two-photon pulsed excitation and time-resolved fluorescence techniques. The pressure dependence of the eigenvalues of the rate matrix yields very rapid rate coefficients of 2.6 ± 0.2 × 10 − 9 cm 3 / ( atom s ) for He and 5.2 ± 0.4 × 10 − 10 cm 3 / ( atom s ) for Ar, about two–three times faster than for the Cs 7 2 D 5 / 2 ⇌ 7 2 D 3 / 2 relaxation. The quenching rates are also rapid, 1.07 ± 0.04 × 10 − 10 cm 3 / ( atom s
Pulsed excitation on the two-photon Cs $6{\phantom{\rule{0.16em}{0ex}}}^{2}{S}_{1/2}\ensuremath{\rightarrow}7{\phantom{\rule{0.16em}{0ex}}}^{2}{D}_{3/2,5/2}$ transition results in time-resolved fluorescence at 697 and 672 nm. The rates for fine-structure mixing between the 72D3/2,5/2 states have been measured for helium and argon rare-gas collision partners. The mixing rates are very fast, $1.26\ifmmode\pm\else\textpm\fi{}0.05\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9} {\mathrm{cm}}^{3}$/atom s for He and $1.52\ifmmode\pm\else\textpm\fi{}0.05\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}10} {\mathrm{cm}}^{3}$/atom s for Ar, driven by the small energy splitting and large radial distribution for the valence electron. The quenching rates are considerably slower, $6.84\ifmmode\pm\else\textpm\fi{}0.09\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}11}$ and $2.65\ifmmode\pm\else\textpm\fi{}0.04\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}11} {\mathrm{cm}}^{3}$/atom s for He and Ar, respectively. The current results are placed in context with similar rates for other alkali-metal--rare-gas collision pairs using adiabaticity arguments.
By applying the laser absorption and fluorescence method,the cross sections for the fine structure mixing and quenching of the Cs(6P) state,induced by collision with He atoms,have been measured.Cesium atoms were optically excited to the 6P3/2 state.The excited atom density and spatial distribution were mapped by monitoring the absorption of a counterpropagating single mode laser beam,which was tuned to the 6PJ→8S1/2 transitions.The effective radiative rates were calculated for the 6PJ→6S transitions.The fluorescence intensity I895 of the sensitized 6P1/2→6S1/2 emission was measured as a function of He density in the range 0.5×1018～4×1018cm-3 at constant temperature T=337 K.It was found that the quantity N/I895 exhibited a parabolic dependence on N,confirming that the quenching of the 6PJ states was due to collision with He atoms,not ground state Cs atoms.The coefficients of the second-order polynomial fitted through the measured data yielded the cross sections σ3/2→1/2=(1.46±0.51)×10-19 cm2 and σD=(2.28±0.80)×10-18 cm2 for the 6PJ fine structure mixing and quenching,respectively,due to collision with He atoms.
Cross sections for the transfer of excitation between fine-structure sublevels of the 9D state of caesium due to collisions with noble-gas atoms are measured. The experimental method employs stepwise excitation with a pulsed dye laser in the second step (6 2 P 3/2 to 9 2 D 5/2 ) and time-resolved detection of sensitised fluorescence 9 2 D 3/2 to 6 2 P 1/2 . The cross sections for the process Cs(9 2 D 3/2 )+A to Cs(9 2 D 5/2 )+A are (in units of 10 -14 cm 2 ) 7.6(1.5), 2.5(5), 2.7(5), 3.0(6) and 3.2(6) for A=He, Ne, Ar, Kr and Xe, respectively. For all the noble gases except helium the experimental cross sections are a few times smaller than the ones obtained in a recent semiclassical calculation.
Applying the cw laser absorption and fluorescence method the cross sections for the fine-structure mixing and quenching of the caesium 5D J states have been measured in pure caesium vapour. Caesium atoms were optically excited to the 5D 5/2 state via the quadrupole-allowed 6S 1/2 →5D 5/2 transition. The ground-state caesium density N 0 , obtained from the absorption at the pumped quadrupole transition, and the fluorescence intensity I 689 of the sensitized 5D 3/2 →6S 1/2 emission were measured simultaneously in the range 3×10 14 cm -3 ⩽ N 0 ⩽1×10 16 cm -3 at constant temperature T = 585 K. It was found that the quantity N 0 2 / I 689 exhibited a parabolic dependence on N 0 , confirming that the quenching of the Cs 5D J states is due to collisions with Cs ground-state atoms, not molecules. The coefficients of the second-order polynomial fitted through the measured data yielded the cross sections σ 5/2→3/2 = (57±19)×10 -16 cm 2 and σ D = (35±10)×10 -16 cm 2 for the Cs 5D J fine-structure mixing and quenching, respectively, due to collisions with caesium ground-state atoms. Using recently calculated Cs*+Cs potentials we performed an analysis which shows good agreement between the measured values and the theoretical predictions.
We report the results of a series of pulsed and cw laser experiments which measure spontaneous and effective lifetimes of the Cs(5DJ) levels and investigate excitation-transfer collisions involving Cs(5DJ) atoms and ground-state-cesium perturbers. With cw excitation of the dipole-forbidden but electric-quadrupole-allowed 6S1/2\ensuremath{\rightarrow}5D5/2 transition, we monitor the ratio of sensitized to direct fluorescence, i.e., I5D3/2\ensuremath{\rightarrow}6P1/2/I5D5/2\ensuremath{\rightarrow}6P3/2. A rate-equation analysis of these data yields values for the Cs(5D5/2)+Cs(6S)\ensuremath{\rightarrow}Cs(5D3/2)+Cs(6S) excitation-transfer rate, and for the rate of quenching of Cs(5D) by ground-state perturbers. The role of out-of-multiplet quenching is discussed at length, and we have demonstrated that quenching by ground-state atoms dominates over that by cesium dimers under these conditions. In the pulsed-laser experiments, the temporal evolution of the 5DJ\ensuremath{\rightarrow}6S and cascade 6PJ\ensuremath{'}\ensuremath{\rightarrow}6S fluorescence was observed following either direct forbidden-line pumping of one fine-structure level, or indirect excitation of both fine-structure levels (i.e., molecular excitation followed by predissociation). Analysis of the buildup and decay rates of the various levels as a function of cesium density yields values for the natural lifetimes of the Cs(5DJ) levels, as well as for the excitation transfer and quenching rates. Best values for the lifetimes and cross sections for Cs-Cs collisions obtained from these combined experiments are \ensuremath{\tau}5D=1250\ifmmode\pm\else\textpm\fi{}115 ns, \ensuremath{\sigma}5/2\ensuremath{\rightarrow}3/2=36\ifmmode\pm\else\textpm\fi{}8 \AA{}2, and \ensuremath{\sigma}5D=30\ifmmode\pm\else\textpm\fi{}3 \AA{}2. In addition, numbers for the 6P level-quenching cross sections due to collisions with Cs atoms and Cs2 molecules, respectively, were obtained: \ensuremath{\sigma}6P(Cs)=6.6\ifmmode\pm\else\textpm\fi{}3.0 \AA{}2 and \ensuremath{\sigma}6P(Cs2)=863\ifmmode\pm\else\textpm\fi{}260 \AA{}2. In the discussion, we show how these new values can be used to reconcile the seemingly discrepant results of several previous studies.
Applying the cw laser fluorescence method, the cross sections for the fine structure mixing and quenching of the Cs 6P state, induced by collisions with ground-state caesium atoms and molecules, have been measured. Caesium atoms were optically excited to the 5D J states via quadrupole-allowed 6S 1/2 5D J transitions, while the resonance states were populated by the radiative and collisional 5D J 6P J transitions. The relative populations of the Cs 6P J sublevels, as well as ratio of the 5D 3/2 to 6P 3/2 populations, were measured as a function of the caesium ground-state number density. From these measurements we obtained the cross section of (14±5) × 10 -16 cm 2 at T = 585 K for the process Cs(6P 1/2 ) Cs(6P 3/2 ) induced by collisions with ground-state caesium atoms. The applied experimental approach enabled the determination of the effective spontaneous rates for the 6P J states which are in agreement with the predictions of Holstein's theory. The cross sections for quenching of 6P J by caesium atoms and molecules were measured at T = 635 K and the obtained values are (1.6±1.4) × 10 -16 cm 2 and (1210±260) × 10 -16 cm 2 , respectively. Using recently calculated Cs*+Cs potentials we performed an analysis which shows a good agreement between the measured values and the theoretical estimates.