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Journal of the Optical Society of America B

Method to measure excited-level-to-excited-level branching ratios and atomic transition probabilities by time-resolved laser photoionization spectroscopy

Scott E. Bisson, B. Comaskey, Earl F. Worden

Published Feb 1, 1995• 8 citations
Publisher

Abstract

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.

DOI
10.1364/josab.12.000193

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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
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.
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.
Laser-induced photoionization and fluorescence signals were simultaneously observed in atomic uranium using a single Nd:YAG-pumped dye laser. These signals were recorded in two specific cases. In the first case, the dye laser was resonant to the first-step transition (0–16900.38 cm−1). In the second case, the laser was near-resonant to the first-step transition with a slight detuning (0.15 cm−1) so that it became two-photon resonant at 33801.06 cm−1. The uranium atoms in the ground state were ionized by a single-color, three-photon photoionization technique resulting in the photoionization signal, and the fluorescence signal was simultaneously obtained from the first excited state involved in the photoionization process. The photoionization and the fluorescence signals in the above-mentioned cases were also estimated theoretically for several values of the photoionization cross section for the transition between the second excited state at 33801.06 cm−1 and the autoionization state at 50701.59 cm−1 using density matrix formalism. From the comparison of theoretically calculated ratios of fluorescence signals in the two specific cases with the experimentally obtained values, the photoionization cross section for the 33801.06–50701.59 cm−1 transition has been obtained, which is found to be (5±1)×10−16 cm2.
This paper reports measurements of the room-temperature laser transition cross section of Nd+3{\mathrm{Nd}}^{+3}Nd+3 in yttrium aluminum garnet at 1.06 \ensuremath{\mu}. One method used is based on the measured upper-state lifetime and a determination of the fluorescence branching ratio for this state. The value thus determined is 3.5\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}19}$ cm2{\mathrm{cm}}^{2}cm2. The second method involves measurement of the ratio of fluorescent intensities from the upper laser level to the ground state and to the lower laser level, and measurement of the cross section in absorption of the transition which involves the ground state. The second method yields a value of 2.7\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}19}$ cm2{\mathrm{cm}}^{2}cm2. The difference represents the contribution of fluorescence to high-lying levels (not included in the determination of branching ratio) and nonradiative transitions. The probable experimental accuracy in both methods is \ifmmode\pm\else\textpm\fi{}15%.
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.