Using the phase-shift technique to measure excited-state lifetimes, upper limits of 1.5 × 10−14 cm3/sec and 3 × 10−14 cm3/sec have been established for the Cs(62P1/2re3/2) + He → Cs(62S1/2) + He quenching rate constants at 350° and 820°K. (In “cross-section” units these are equivalent to 10−19 cm2 upper limits.) The natural lifetimes were measured to be 30.8 ± 1.5 × 10−9 sec and 35.2 ± 1.5 × 10−9 sec for the Cs 62P3/2 and 62P1/2 states.
Using the phase-shift technique to measure excited-state lifetimes, upper limits of 1.5 × 10−14 cm3/sec and 3 × 10−14 cm3/sec have been established for the Cs(62P1/2re3/2) + He → Cs(62S1/2) + He quenching rate constants at 350° and 820°K. (In “cross-section” units these are equivalent to 10−19 cm2 upper limits.) The natural lifetimes were measured to be 30.8 ± 1.5 × 10−9 sec and 35.2 ± 1.5 × 10−9 sec for the Cs 62P3/2 and 62P1/2 states.
The effects of imprisonment of resonance radiation in potassium vapor and of collisions between excited potassium atoms and N2, H2, HD, and D2 molecules, on the measured lifetimes of the 42P states, have been investigated by the method of delayed coincidences. The potassium atoms were excited with short pulses of resonance radiation, and the delays between the exciting and fluorescent pulses were measured with a time-to-amplitude converter. At pure potassium densities below 1010 atoms/cm3, the measured lifetimes approach the constant values 27.8 ± 0.8 and 27.6 ± 0.8 ns, corresponding to the natural lifetimes of the 42P1/2 and 42P3/2 states, respectively. At higher densities the effective lifetimes are in satisfactory agreement with the predictions of Holstein's theory. The decrease in the measured decay rates observed upon addition of the diatomic gases yielded cross sections for quenching collisions with N2, H2, HD, and D2 which equal 34.0 ± 2.0 Å2, 9.4 ± 1.3 Å2, 11.9 ± 1.5 Å2, and 8.0 ± 2.0 Å2, respectively.
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.
Mixing cross sections of Cs between the 62P1/2 and 62P3/2 levels and quenching cross sections from these levels to the ground state 62S1/2 were measured, with methane, ethane, and propane as collision partners. We excited Cs to the 6P3/2 level with a tunable nanosecond pulse laser and measured the fluorescence at the 62P1/2 level. The measured mixing cross sections with methane, ethane, and propane were (1.39 ± 0.16), (5.67 ± 0.85), and (7.91 ± 0.93)×10−15 cm2, respectively, and the statistically averaged quenching cross sections were (1.5 ± 0.25), (10 ± 2.0), and (25 ± 5.3)×10−18 cm2, respectively. The quenching cross section of Cs-propane is reported for the first time.
6 2P1/2 ↔ 6 2P3/2 mixing and 6 2S1/2 ← 6 2P1/2,3/2 quenching in cesium, induced in collisions with ground state N2, H2, HD, and D2 molecules, have been investigated using techniques of sensitized fluorescence. Mixtures of cesium vapor and the gases, in which the cesium vapor pressure was kept very low to avoid multiple scattering, were irradiated with each component of the cesium resonance doublet in turn. The fluorescence which contained both components of the doublet was observed in a direction perpendicular to that of the exciting beam. Measurements of the relative intensities of the fluorescent components yielded the following cross sections for mixing and quenching. For Cs–N2 collisions: Q12(2P1/2 → 2P3/2) = 4.7 Å2, Q21(2P1/2 ← 2P3/2) = 25 Å2, Q10(2S1/2 ← 2P1/2) = 77 Å2, Q20(2S1/2 ← 2P3/2) = 69 Å2. For Cs–H2 collisions: Q12 = 6.7 Å2, Q21 = 44 Å2, Q10 = 7 Å2, Q20 = 5 Å2. For Cs–HD collisions: Q12 = 4.8 Å2, Q21 = 32 Å2, Q10 = 4 Å2, Q20 = 3 Å2. For Cs–D2 collisions: Q12 = 4.2 Å2, Q21 = 28 Å2, Q10 = 8 Å2, Q20 = 7 Å2. The Cs–N2 and Cs–H2 cross sections supersede the values published previously (McGillis and Krause 1967). The cross sections Q21 appear to exhibit resonances with molecular rotational transitions.
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.