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Physical Review A

Lifetime measurements of cesium 5d2D5/2,3/2 and 11s2S1/2 states using pulsed-laser excitation

Diana DiBerardino, Carol E. Tanner, A. Sieradzan

Published Jun 1, 1998• 30 citations
Publisher

Abstract

We report measurements of the $5d{}^{2}{D}_{5/2},$ $5d{}^{2}{D}_{3/2},$ and $11s{}^{2}{S}_{1/2}$ state lifetimes in the ${}^{133}$Cs atom to be 1281(9), 909(15), and 351(4) ns, respectively. A pulsed-dye laser selectively excites atomic Cs from the ground state, via a single-photon quadrupole transition, to the $5d$ states and, via a two-photon electric dipole transition, to the $11s$ state. A spectrometer-photomultiplier system detects the fluorescence from the decay of interest and a digitizing oscilloscope records the direct output of the photomultiplier. The data are fit to an exponential function to yield a value for the mean lifetime of the selected state.

DOI
10.1103/physreva.57.4204

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We report measurements of the 5d2D5/2,5d{}^{2}{D}_{5/2},5d2D5/2​, 5d2D3/2,5d{}^{2}{D}_{3/2},5d2D3/2​, and 11s2S1/211s{}^{2}{S}_{1/2}11s2S1/2​ state lifetimes in the 133{}^{133}133Cs atom to be 1281(9), 909(15), and 351(4) ns, respectively. A pulsed-dye laser selectively excites atomic Cs from the ground state, via a single-photon quadrupole transition, to the 5d5d5d states and, via a two-photon electric dipole transition, to the 11s11s11s state. A spectrometer-photomultiplier system detects the fluorescence from the decay of interest and a digitizing oscilloscope records the direct output of the photomultiplier. The data are fit to an exponential function to yield a value for the mean lifetime of the selected state.
We measure the lifetime of the cesium 52D5/25^{2}D_{5/2}52D5/2​ state using a time-resolved single-photon-counting method. We excite atoms in a hot vapor cell via an electric quadrupole transition at a wavelength of 685 nm and record the fluorescence of a cascade decay at a wavelength of 852 nm. We extract a lifetime of 1353(5)1353(5)1353(5) ns for the 52D5/25{\phantom{\rule{0.16em}{0ex}}}^{2}{D}_{5/2}52D5/2​ state, in agreement with a recent theoretical prediction. In particular, the observed lifetime is consistent with the literature values of the polarizabilities of the cesium 6P6P6P states. Our measurement contributes to resolving a long-standing disagreement between a number of experimental and theoretical results.
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.
We present lifetime measurements of the 5D3∕25{D}_{3∕2}5D3∕2​ and 5D5∕25{D}_{5∕2}5D5∕2​ states of rubidium using the time-correlated single-photon-counting method. We perform the experiment in a magneto-optical trap of 87Rb^{87}\mathrm{Rb}87Rb atoms using a two-step excitation with the trap laser at 780nm780\phantom{\rule{0.3em}{0ex}}\mathrm{nm}780nm as the first step. We record the 761.9nm761.9\phantom{\rule{0.3em}{0ex}}\mathrm{nm}761.9nm fluorescence from the decay of the 5D3∕25{D}_{3∕2}5D3∕2​ state to the 5P1∕25{P}_{1∕2}5P1∕2​ state, and measure the lifetime of the 5D3∕25{D}_{3∕2}5D3∕2​ state $\ensuremath{\tau}=246.3(1.6)\phantom{\rule{0.3em}{0ex}}\mathrm{ns}$. We record the 420.2nm420.2\phantom{\rule{0.3em}{0ex}}\mathrm{nm}420.2nm fluorescence from the cascade decay of the 5D5∕25{D}_{5∕2}5D5∕2​ state to the 5S1∕25{S}_{1∕2}5S1∕2​ state through the 6P3∕26{P}_{3∕2}6P3∕2​ state, and extract the lifetime of the 5D5∕25{D}_{5∕2}5D5∕2​ state $\ensuremath{\tau}=238.5(2.3)\phantom{\rule{0.3em}{0ex}}\mathrm{ns}$.
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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.