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Optics Letters

Autoionizing decay rates measured by optical nutation

A. V. Smith, T. D. Raymond

Published Feb 15, 1991• 3 citations
Publisher

Abstract

Using a single-mode pulsed laser we have measured autoionizing lifetimes for the 3p' (3)D states of atomic oxygen by measuring the dependence of ionization on the fluence of light driving the 3s' (3)D-3p' (3)D transition. From the frequency of the Rabi oscillations we deduce transition strengths, and from the modulation depth we calculate ionization lifetimes. These are to our knowledge the first measurements of these quantities for these transitions.

DOI
10.1364/ol.16.000267

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Using a single-mode pulsed laser we have measured autoionizing lifetimes for the 3p' (3)D states of atomic oxygen by measuring the dependence of ionization on the fluence of light driving the 3s' (3)D-3p' (3)D transition. From the frequency of the Rabi oscillations we deduce transition strengths, and from the modulation depth we calculate ionization lifetimes. These are to our knowledge the first measurements of these quantities for these transitions.
A transform-limited light pulse from a tunable laser can be used to measure atomic lifetimes much shorter or much longer than the light puke duration by measuring linewidths in the case of short lifetimes or decay rates in the case of long lifetimes. However, when the atomic lifetime is comparable to the duration of the exciting pulse, these methods are difficult to apply. We demonstrate that, for the latter case, an optical nutation measurement yields both lifetimes and transition strengths with high accuracy. We prepare oxygen atoms in a single angular momentum state (J, mj) in a collision-free and Doppler-free environment.
The oscillator strength of the (6s6p)3{)\mathrm{}}^{3})3P1{P}_{1}P1​-(6s7s)1{)\mathrm{}}^{1})1S0{S}_{0}S0​ transition and the lifetime of the (6s7s)1{)\mathrm{}}^{1})1S0{S}_{0}S0​ state in 174Yb^{174}\mathrm{Yb}174Yb have been measured to be (8.0\ifmmode\pm\else\textpm\fi{}1.6)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}4}$ and 45.8\ifmmode\pm\else\textpm\fi{}1.0 nsec, respectively. The former value was obtained by use of coherent optical techniques (optical nutation and ac Stark splitting), while the latter was obtained by monitoring cascade fluorescence following pulsed excitation.
We have used two methods to measure the oscillator strength of the transition between the ground and 17992 cm-1 level in 174Yb. The first technique involves exciting the transition with a laser pulse that is nearly time-bandwidth limited, of uniform intensity, and has a reproducible shape from shot to shot. The population left in the excited state after the pulse varies sinusoidally with a period that depends on the integral over time of the electric field amplitude and the transition oscillator strength. These are the Rabi oscillations that are predicted by application of the Schrodinger equation to the two-level atom. The excited-state population is probed using a two-step photoionization to the continuum. The electric field amplitude is determined from the temporal profile and the intensity of the laser pulse. The second method involves observation of the polarization rotation of a set of degenerate sublevels brought about by a time-bandwidth limited light-shift laser. One sublevel (mj = 0) of the J = 1 level at 17992 cm-1 is populated by a linearly polarized laser. A second copropagating light-shift laser, which is linearly polarized at an angle to the first laser, is tuned between 7.5 and 30 GHz off-resonance with the transition. The light-shift laser causes population to be promoted into the mi = ±1 levels by a virtual transition through the ground J = 0, = 0 level. Two linearly polarized photoionizing lasers photoionize the population only from the mi = ±1 levels. The photoion signal oscillates sinusoidally with a period that depends only on the integrated pulse intensity, the laser detuning, and the transition oscillator strength.
We study, using a combination of experiment and theory, the excitation and decay of very-high-$n\phantom{\rule{4pt}{0ex}}(n\ensuremath{\sim}280\text{--}430)$ strontium autoionizing Rydberg states formed by near-resonant driving of the $5s\phantom{\rule{0.16em}{0ex}}^{2}S_{1/2}\ensuremath{\rightarrow}5p\phantom{\rule{0.16em}{0ex}}^{2}P_{1/2}$ core-ion transition. The branching ratio between decay through radiative transitions and through autoionization is explored. Autoionization rates are measured as a function of both the nnn and $\ensuremath{\ell}$ quantum numbers of the Rydberg electron. The nonstationary decay dynamics is studied by creating and manipulating Rydberg wave packets and by varying the laser pulse that drives the core excitation.
The use of autoionization as a tool to quantitatively analyze transitions between high-n strontium Rydberg states with low-to-intermediate values of L is described and is demonstrated through observations of Rabi oscillations when driving 5snf 1F3 → 5s(n + 1)g 1G4, 5snf 1F3 → 5s(n + 2)h 1H5, and 5snp 1P1 → 5s(n + 1)d 1D2 transitions using microwave fields. The technique is shown to offer advantages when compared to selective field ionization and can be used with other alkaline-earth and alkaline-earth-like metals.