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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Measurement Of Atomic Oscillator Strengths Using Pulsed Single-Frequency Dye Lasers

C. Haynam, B. Comaskey, Michael Austin Johnson, Jeffrey A. Paisner, Earl F. Worden

Published Jun 22, 1988• 2 citations
Publisher

Abstract

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.

DOI
10.1117/12.945525

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•Jan 1, 1987•1 citation

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Two-photon Resonant Excitation Of Thallium In An Atomic Beam (multiphoton, Radiative Lifetimes).

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We have observed fluorescence and ionization signals resulting from two-photon resonant excitation of thallium in an atomic beam. The output of a pulsed dye laser is used to excite the resonance between the ground state (6('2)P(,1/2)) and an excited n('2)P state of thallium. Both two-photon absorption and three-photon absorption occur simultaneously; the latter results in photoionization of the atom. The excited states populated by two-photon absorption decay via cascade fluorescence back to the ground state; one or more of these spectral components constitute our fluorescence signal. The lifetimes of the excited n('2)P states of thallium have been measured directly by observing the exponential decay of this fluorescence. Calculations are included to ascertain the time required for the fluorescence signal to reach within 2% of a simple exponential decay. This decay is a measure of the lifetime of the initial state, under the condition that none of the fluorescence components arise from states which are populated by cascade through longer-lived states. The lifetimes of the n('2)P(,1/2) and n('2)P(,3/2) states of thallium for n = 7 to 11 are determined in this manner and compared with the values deduced from semi-empirical calculations of oscillator strengths by various authors. For calculations employing the effects of core polarizability in the electron wavefunctions and in the transition matrix elements, the agreement is very good--to within our experimental uncertainty, which is typically(, )<5%. Our measurements are also compared to the four other known experimental values for such excited states of thallium. Some of these previous experiments and calculations were carried out in conjunction with parity non-conservation experiments in thallium. Our measurements may provide useful checks on the accuracy of some of the calculations performed in the evaluation of such experiments. The ionization and fluorescence signals are also studied under conditions of strong saturation of the two-photon resonance with the 7('2)P states. The manifestation of saturation in the ionization signal is a broadening of the excitation spectrum, which is found to greatly exceed that of the fluorescence signal. Furthermore, the ratio of the ionization signal to the fluorescence signal at the peak of the resonance is found to vary linearly at intensities below about 10('9) W/cm('2); this too saturates at higher intensities. Various models are employed to simulate the observed behavior, encompassing both rate equations as well as density matrix formulations. The numerical solutions to these models are compared with the observed behavior; the agreement is found to depend strongly on the assumed experi- mental conditions to which the ensemble of atoms is subjected.

•Jan 1, 1986•0 citations
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.
Two methods have been used to measure the oscillator strength of the transition between the ground and 17,992 cm level in XUYb. 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 second method involves observation of the polarization rotation of a set of degenerate sublevels brought about by a light-shift laser. One sublevel (m/sub j/ = 0) of the J = 1 level at 17,992 cm 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 m/sub j/ = +-1 levels through the virtual J = 0, m/sub j/ = 0 level. Two linearly polarized photoionizing lasers photoionize the population only from the m/sub j/ = +-1 levels. The photoion signal oscillates cosinusoidally with a period that depends only on the integrated pulse intensity, the laser detuning, and the transition oscillator strength. Finally, polarization selectivity has been shown experimentally to allow selective photoionization of the odd isotopes of ytterbium using broadband lasers.
The theory of a new method to measure oscillator strengths is presented. The method exploits the ac Stark interaction of a laser pulse detuned from a transition between an initially populated state a and a second state b of an atom. We assume the density matrix \ensuremath{\rho} of state a initially has only diagonal elements given by 〈m\ensuremath{\Vert}\ensuremath{\rho}\ensuremath{\Vert}m〉=C+Dm2{\mathrm{Dm}}^{2}Dm2 where C and D\ensuremath{\ne}0 are constants and m is the Zeeman sublevel quantum number. The laser pulse is linearly polarized along an axis different from the quantization axis and therefore rearranges the atoms among the various Zeeman sublevels. Changes of the relative Zeeman sublevel populations induced by the laser pulse can be readily detected by monitoring changes in the angular distribution or polarization of fluorescent light emitted when the atoms radiatively decay to some final state f. This paper considers the general problem where states a, b, and f have arbitrary angular momentum. We derive the functional dependence of the polarized fluorescent light fluence on the laser pulse fluence (pulse energy per unit area).For spatially uniform laser pulses, these signals are periodic functions of the laser fluence. When the laser is completely speckled, we show that the signal is well approximated by a Lorentzian curve. This latter case is of considerable experimental interest since most pulsed dye lasers have poor transverse mode structure which can readily be converted into a statistically well-defined speckle pattern. The oscillator strength of the transition between states a and b is found using (1) the fluence half-width of the ``depolarization curve,'' the Lorentzian-like dependence of the fluorescence polarization on the laser pulse fluence, (2) the detuning of the laser from the transition frequency ${\ensuremath{\omega}}_{\mathrm{ab}}$, and (3) some known constant factors which depend on the angular momenta of states a, b, and f. The physics of the situation is very similar to that of the conventional hook method with this difference: the roles of the atoms and the photons have been interchanged. We therefore call this new method the inverse hook method. The inverse hook method is relatively insensitive to the details of the atomic absorption line shape and also to the temporal and spatial profile of the laser pulse. It yields absolute oscillator strengths and it is especially suitable for measurements of transitions between excited atomic states, including autoionizing states.
An established photoionization branching-ratio measurement method, in which an excited level of an atom is populated by a pulsed laser from the ground level and repopulation of the ground level is measured by a second laser or lasers, is extended to the case with a finite lower-level lifetime. Two pulsed dye lasers populate the upper and the lower levels of the transition of interest. A third pulsed dye laser probes the time evolution of the lower level by a photoionization process. This measurement, coupled with the upper- and the lower-level lifetimes, permits the determination of the branching ratio and transition probability. Cerium branching ratios obtained are compared with those that we determined from the emission spectrum of cerium. The method is tested for the difficult case in which the lifetimes of the transition levels are nearly equivalent. The effects of magnetic sublevels are investigated in ytterbium.
When internal states of atoms are manipulated using coherent optical or radio-frequency (rf) radiation, it is essential to know the polarization of the radiation with respect to the quantization axis of the atom. We first present a measurement of the two-dimensional spatial distribution of the electric-field amplitude of a linearly polarized pulsed rf electric field at $\ensuremath{\sim}25.6\phantom{\rule{0.28em}{0ex}}\mathrm{GHz}$ and its angle with respect to a static electric field. The measurements exploit coherent population transfer between the 35s35s35s and 35p35p35p Rydberg states of helium atoms in a pulsed supersonic beam. Based on this experimental result, we develop a general framework in the form of a set of equations relating the five independent polarization parameters of a coherently oscillating field in a fixed laboratory frame to Rabi rates of transitions between a ground and three excited states of an atom with arbitrary quantization axis. We then explain how these equations can be used to fully characterize the polarization in a minimum of five Rabi-rate measurements by rotation of an external bias field, or, knowing the polarization of the driving field, to determine the orientation of the static field using two measurements. The presented technique is not limited to Rydberg atoms and rf fields but can also be applied to characterize optical fields. The technique has the potential for sensing the spatiotemporal properties of electromagnetic fields, e.g., in metrology devices or in hybrid experiments involving atoms close to surfaces.
In an experiment on three-photon laser excitation 5S 1/2 → 5P 3/2 → 6S 1/2 → 37P 3/2 of a single 87 Rb, Rydberg atom in an optical dipole trap, we have observed for the first time three-photon Rabi oscillations between the ground and the Rydberg states. A single atom was detected optically by resonance fluorescence signal using a low-noise sCMOS video camera. The relative probability for the atom to remain in the trap after the action of three synchronized exciting laser pulses with durations varying from 100 ns to 2 µs was measured. A distinctive feature of the experiment was the use of intense laser radiation with a wavelength of 1367 nm at the second excitation step, providing a single-photon Rabi frequency up to 2 GHz to control the effective detunings of intermediate levels of the three- photon transition due to the dynamic Stark effect. Rabi oscillations with frequencies from 1 to 5 MHz were registered depending on the intensity of laser pulses of the first and second excitation steps with coherence time 0.7–0.8 µs. Ways to increase the coherence time and contrast of three-photon Rabi oscillations for applications in quantum information with Rydberg atoms are discussed.
We have observed fluorescence and ionization signals resulting from two-photon resonant excitation of thallium in an atomic beam. The output of a pulsed dye laser is used to excite the resonance between the ground state (6('2)P(,1/2)) and an excited n('2)P state of thallium. Both two-photon absorption and three-photon absorption occur simultaneously; the latter results in photoionization of the atom. The excited states populated by two-photon absorption decay via cascade fluorescence back to the ground state; one or more of these spectral components constitute our fluorescence signal. The lifetimes of the excited n('2)P states of thallium have been measured directly by observing the exponential decay of this fluorescence. Calculations are included to ascertain the time required for the fluorescence signal to reach within 2% of a simple exponential decay. This decay is a measure of the lifetime of the initial state, under the condition that none of the fluorescence components arise from states which are populated by cascade through longer-lived states. The lifetimes of the n('2)P(,1/2) and n('2)P(,3/2) states of thallium for n = 7 to 11 are determined in this manner and compared with the values deduced from semi-empirical calculations of oscillator strengths by various authors. For calculations employing the effects of core polarizability in the electron wavefunctions and in the transition matrix elements, the agreement is very good--to within our experimental uncertainty, which is typically(, )<5%. Our measurements are also compared to the four other known experimental values for such excited states of thallium. Some of these previous experiments and calculations were carried out in conjunction with parity non-conservation experiments in thallium. Our measurements may provide useful checks on the accuracy of some of the calculations performed in the evaluation of such experiments. The ionization and fluorescence signals are also studied under conditions of strong saturation of the two-photon resonance with the 7('2)P states. The manifestation of saturation in the ionization signal is a broadening of the excitation spectrum, which is found to greatly exceed that of the fluorescence signal. Furthermore, the ratio of the ionization signal to the fluorescence signal at the peak of the resonance is found to vary linearly at intensities below about 10('9) W/cm('2); this too saturates at higher intensities. Various models are employed to simulate the observed behavior, encompassing both rate equations as well as density matrix formulations. The numerical solutions to these models are compared with the observed behavior; the agreement is found to depend strongly on the assumed experi- mental conditions to which the ensemble of atoms is subjected.