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Physical Review A

Two-photon-resonance effect in atomic-uranium experiments

C. S. Chang, Robert E. Schlier

Published Mar 1, 1980• 6 citations
Publisher

Abstract

The authors investigate resonant two-step laser excitation in a cascade three-level system using an atomic-uranium beam. Both single-photon and two-photon processes are studied by varying the time delay between the two different excitation pulses. The experimental data are compared to the results of simple theoretical models. The calculations include the effects of the magnetic sublevels. The major theoretical prediction of a two-photon resonance is verified experimentally by using simultaneous irradiation from two lasers. The agreement between theory and experiment is found to be satisfactory.

DOI
10.1103/physreva.21.872

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Journal of Physics B Atomic and Molecular Physics•Jan 28, 1987•7 citations
The authors investigate resonant two-step laser excitation in a cascade three-level system using an atomic-uranium beam. Both single-photon and two-photon processes are studied by varying the time delay between the two different excitation pulses. The experimental data are compared to the results of simple theoretical models. The calculations include the effects of the magnetic sublevels. The major theoretical prediction of a two-photon resonance is verified experimentally by using simultaneous irradiation from two lasers. The agreement between theory and experiment is found to be satisfactory.
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.
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.
For the pair of 238U^{238}\mathrm{U}238U levels at 3868 and 26 558 ${\mathrm{cm}}^{\ensuremath{-}1}$0, the upper-state population was measured as a function of the irradiance of a resonant exciting pulse of fixed duration. The observed damped Rabi flopping showed that the two-level system was partially coherently excited. The results were compared with the prediction of an exact solution of the time-dependent Schr\"odinger equation for two-level systems excited by a detuned rectangular pulse. The Schr\"odinger equation solution, after averaging over laser irradiance fluctuations, agrees well with the data.
We have theoretically and experimentally investigated the laser-detected magnetic resonance induced by radio-frequency two-photon processes in Fg=4{F}_{g}=4Fg​=4 of D1{D}_{1}D1​ line of cesium atoms. The effective Hamiltonian for the interaction between the two radio-frequency magnetic fields and sublevels at the ground state of Fg=4{F}_{g}=4Fg​=4 is derived. By appropriately selecting the frequencies of the two radio-frequency fields, the Raman two-photon process and the cascade two-photon process can occur, which induce the magnetic resonance detected through laser transmission spectra. The theoretical calculation results fit well with the experimental data. Our results maybe apply for measuring the high bandwidth radio-frequency magnetic fields in space and studying the magnetic-induction tomography.
By means of a simple theoretical model and experimental results, we analyse the two-photon ionization of cold rubidium atoms. We consider a two-step process in which ground state atoms are ionized by two blue (421 nm) photons, chosen to be quasi-resonant with the 5S → 6P transition. We show that for a good description of the process we have to take into account not only the three states coupled by the laser radiation, but also all the atomic states involved in the spontaneous emission cascade from the 6P to the 5S state, since optical pumping from 5S 1/2 ( F = 2) to the 5S 1/2 ( F = 1) states modifies the ionization efficiency when ionizing near resonance. The experimental and theoretical determination of ionization cross sections for excitations near resonance with the 6P 1/2 and the 6P 3/2 intermediate levels is presented.
For pt.I see ibid., vol.20, p.251 (1987). Theoretical expressions for cascade light intensity as a function of time have been evaluated for the case of cascade Zeeman beats produced by two-step excitation with broad-line laser pulses, and the results are compared with experimentally observed cascade Zeeman beats in Fe I. The beats were detected in time-resolved fluorescence from intermediate levels populated by cascades from highly excited levels of Fe I, using three different stepwise-excitation-cascade sequences. In the case of coincident laser pulses, good agreement between theory and experiment is obtained over a range of magnetic fields when allowance is made for Larmor precessions during the excitation period, for the width and shape of the exciting laser pulses and for the contribution of impurity processes. The effects of precession during the excitation period are especially important for the excitation sequence a 5 D 4 to z 5 F degrees 5 to e 5 F 5 , for which short-pulse theories predict no quantum beats for the experimental geometry used (parallel linear polarisations in the two excitation steps). For non-coincident pulses a predicted oscillation in the amplitude of the cascade beats with magnetic field has also been observed.