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Applied Physics B

Understanding photoexcitation dynamics in a three-step photoionization of atomic uranium and measurement of photoexcitation and photoionization cross sections

P. K. Mandal, A. C. Sahoo, R. C. Das, M.L. Shah, A. K. Pulhani, K. G. Manohar, Vas Dev

Published Aug 3, 2015• 7 citations
Publisher
DOI
10.1007/s00340-015-6192-z

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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.
The dynamical process of photoexcitation and photoionization of alkali atoms is studied with three-step laser pulses, focusing on the similarities and differences between Li and Cs atoms on their properties by making a comparison of them. Based on several excitation schemes, the present work not only establishes the rate equations of atom population for all related transition states, but also obtains the analytical solutions of photoexcitation and photoionization process. The mathematical solutions are simplified significantly by restricting the most general case to the several special cases, either designed or selected carefully, in order to highlight the main factors and obtain the physical insight underlying the complicated mathematical expressions. With self-programming, the possible impact of time configuration of laser pulses on the three-step laser excitation process of the photoexcitation and photoionization is calculated and studied systematically. Variation of the ionization efficiency with the laser parameters is investigated and discussed. With the same time configuration of laser pulses, the dependences of atom population for all the related transition states on the two different excitation paths are compared and analyzed, reflecting the impact of changing the atomic parameters. Under the similar excitation conditions, the differences of ionization efficiency between Li and Cs atoms are explored. Finally, based on the present study, several means for optimizing ionization efficiency are proposed.
The photoionization cross sections of two even-parity excited states 5d6d3D15d6d\phantom{\rule{0.3em}{0ex}}^{3}D_{1}5d6d3D1​ and 6s7d3D26s7d\phantom{\rule{0.3em}{0ex}}^{3}D_{2}6s7d3D2​ of atomic Ba at the ionization-laser wavelength of 556.6nm556.6\phantom{\rule{0.3em}{0ex}}\mathrm{nm}556.6nm were measured. We found that the total cross section depends on the relative polarization of the atoms and the ionization-laser light. With density-matrix algebra, we show that, in general, there are at most three parameters in the photoionization cross section. Some of these parameters are determined in this work. We also present the measurement of the radiative lifetime of five even-parity excited states of barium.