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Journal of Physics B Atomic and Molecular Physics

Lifetimes, depopulation cross sections and hyperfine structures of some Rydberg S and D states of133Cs

J. S. Deech, Robert Luypaert, Leslie Pendrill, George William Series

Published Apr 1, 1977• 60 citations
Publisher

Abstract

Measurements have been made of time-resolved fluorescence from n 2 S 1/2 and n 2 D 3/2 states of 133 Cs (n=8 to 14) over a range of vapour densities covering the onset of collisional depopulation. Lifetimes for the free atom and depopulation cross sections are deduced. Lifetimes are proportional to (n*) x with x=2.52+or-0.06 (S states) and 2.62+or-0.06 (D 3/2 states). Cross sections are proportional to (n*) 4 . Hyperfine-structure interaction constants for the 2 D 3/2 states determined by the method of quantum beats agree with the recent results of Belin et al. (1976).

DOI
10.1088/0022-3700/10/5/004

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Measurements have been made of time-resolved fluorescence from n 2 S 1/2 and n 2 D 3/2 states of 133 Cs (n=8 to 14) over a range of vapour densities covering the onset of collisional depopulation. Lifetimes for the free atom and depopulation cross sections are deduced. Lifetimes are proportional to (n*) x with x=2.52+or-0.06 (S states) and 2.62+or-0.06 (D 3/2 states). Cross sections are proportional to (n*) 4 . Hyperfine-structure interaction constants for the 2 D 3/2 states determined by the method of quantum beats agree with the recent results of Belin et al. (1976).
Measurements of the time-resolved fluorescence from some highly excited states of 133Cs atoms (n2D3/2, n2D5/2 and n2S1/2(n-4)2F; n=9 to 15) have shown multi-exponential behaviour which depends on vapour pressure. This behaviour is the result of mixing of population caused by collisions between the excited and ground-state atoms. The variation of the exponential rate constants with vapour density yields the free-atom lifetimes and collisional transfer cross sections of these excited states. An analogy is drawn between this variation and that of the energy eigenvalues of an atom under external perturbation.
Cross sections for the disalignment of excited caesium atoms, by collision with atoms in ground states, have been determined by studying the damping of quantum beats in fluorescence. Atoms in a sealed cell were excited selectively to 122D3/2 and 132S3/2 by a pulsed tunable laser and discharge lamp. Alignment was induced by linear polarisation of the exciting light and monitored correspondingly. The quantum beats originate in the coherent excitation of hyperfine states whose structures have been determined in previous work. Collisional damping is investigated studying the quantum-beat signal over a range of atomic densities. The fluorescence contains a component representing the decay of population as well as of alignment, and extraction of the alignment cross sections relies on previous measurements of the depopulation cross sections. The results for disalignment cross sections are: sigma (2)(122D3/2)=4.1+or-0.8*10-16 m2, sigma (2)(132D3/2)=5.3+or-0.9*10-16 m2, about three times larger than the depopulation cross sections. Radiative lifetimes obtained from the analysis agree with previous determinations.
The lifetime r and the cross section a for depopulation induced by collisions with ground-state Rb atoms were measured for the 14 2D3 / 2 state of Rb.The experiment was performed in the gas-cell conditions in a range of Rb vapour temperatures in the vicinity of 340 K.The lifetime value r = 1970(130) ns, agrees with the theoretical prediction with allowance for the influence of blackbody radiation as well as of the effects due to core polarizability and spin-orbit interaction.The measured cross section Q = 6.5(3.1)x 10 -12 cm2 is close to the geometrical cross section.This agrees with similar observations made by other authors for the case of the lower n 2D states of Rb.
The states were studied by selective detection of the fluorescence generated in atoms of the vapour by stepwise excitation, using as sources a conventional caesium lamp for the first step from the ground state and a pulsed, tunable laser for the second. The techniques of delayed coincidence counting were applied to measure the time distribution of intensity of the fluorescent light. The observed modulation, representing in each case a superposition of the hyperfine intervals showed a characteristic period which was interpreted as the reciprocal of the magnetic interaction constant a for the states in question. The relative simplicity of the modulation patterns is a consequence of the negligibly small quadrupole interaction in 133 Cs. With the polarizer oriented at cos -1 3 -1/2 to the analyzer the modulation was suppressed, leaving a simple exponential decay from which the lifetime of the population tau , could be determined.
The hyperfine structure and lifetime of the 6 2 D 3/2 and 6 2 D 5/2 states in 39 K are studied experimentally. The states were excited from the ground state by two-photon absorption of the laser light pulses. The hyperfine-structure intervals, and hence the hyperfine-structure interaction constants, were obtained from the numerical analysis of the zero-field quantum beat signals. The unmodulated component of the fluorescence decay curve served to determine the lifetime. In a separate experiment a magnetic field was applied to induce partial decoupling of the electronic and nuclear angular momenta in the 6 2 D states. The sign of the magnetic dipole interaction constants was deduced from the resulting difference between the intensities of sigma + and sigma - polarised fluorescence.