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Journal of Physics B Atomic Molecular and Optical Physics

Multiphoton ionization of Rb2in the wavelength range 620-670 nm

Hidetoshi Suemitsu, H Kitaura, R Yokoyama, Masahiro Ehara, H. Nakatsuji

Published Nov 14, 1992• 4 citations
Publisher

Abstract

The relative production rates of Rb + and Rb + 2 ions through the multiphoton ionization (MPI) of Rb 2 and the effective order of non-linearity k for these ions were measured in the wavelength range 620-670 nm. The measured results indicated that these ions were produced by two- or three-photon ionization of Rb 2 . The Franck-Condon factors calculated for the transition from the ground state (X 1 Sigma + g ) to the first intermediate state (B 1 Pi u ) were in good agreement with the production rates obtained for Rb + and Rb + 2 ions. From these reasons the authors concluded that in the process of MPI of Rb 2 the transition to the Bu 1 Pi u state plays a crucial role in the production of both ions. The competitive relations between the production processes of Rb + 2 and Rb + ions were derived. In the wavelength range at around 669 nm the ratio of the number of Rb + ions to that of Rb + 2 ions produced through three-photon ionization of Rb 2 was about 4/1.

DOI
10.1088/0953-4075/25/21/017

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The relative production rates of Rb + and Rb + 2 ions through the multiphoton ionization (MPI) of Rb 2 and the effective order of non-linearity k for these ions were measured in the wavelength range 620-670 nm. The measured results indicated that these ions were produced by two- or three-photon ionization of Rb 2 . The Franck-Condon factors calculated for the transition from the ground state (X 1 Sigma + g ) to the first intermediate state (B 1 Pi u ) were in good agreement with the production rates obtained for Rb + and Rb + 2 ions. From these reasons the authors concluded that in the process of MPI of Rb 2 the transition to the Bu 1 Pi u state plays a crucial role in the production of both ions. The competitive relations between the production processes of Rb + 2 and Rb + ions were derived. In the wavelength range at around 669 nm the ratio of the number of Rb + ions to that of Rb + 2 ions produced through three-photon ionization of Rb 2 was about 4/1.
The relative cross sections of the production of Cs + and Cs 2 + ions through the two-photon ionization of Cs 2 were measured in the 5300-6200 Å wavelength range. A linear polarized dye laser was operated in the CW mode as a light source. The results showed that (1) the cross sections for Cs + ions have a broad peak at around 5570 Å and the threshold at around 6010 Å, and (2) those for Cs 2 + ions have the largest peak at around 5940 Å and many structures in the wavelength range longer than it. Through consideration of the above results, we suggested that Cs + ions are produced not only by two-photon ionization of Cs 2 , but also by a participation of a third photon. The threshold for Cs + ions at around 6010 Å is concerned with the intermediate excited-state Cs 2 (C 1 ∏ u + (ν ′ )), which can be excited from the ground state X 1 Σ g + (ν ′′ =0).
Multiphoton ionization (MPI) of barium atom using an excimer-pumped pulsed dye laser has been studied in the wavelength range 570-608 nm at a laser intensity approximately 10.0 GW cm -2 . Resonances in MPI were recorded by monitoring either the ions produced in the multiphoton process using a thermionic detector or fluorescence from the ions formed in their various excited states of Ba + . The observation of photoion and fluorescence spectra were made on Ba vapour in the heat-pipe oven in the moderate-density regime ( approximately 10 13 atoms/cm 3 ) so that the collisional effects are negligible. Fine-structure resolution of the final ionic state (6p 2 P 1/2,3/2 ), produced after four-photon autoionizing decay was obtained. The decay of the Ba atom after four-photon absorption preferentially populates the 6p 2 P 3/2 state relative to the 6p 2 P 1/2 state.
The multiphoton excitation of rubidium has been investigated over the 4600-6500-\AA{} wavelength region with a tunable dye-laser source having a linewidth better than 0.1 \AA{} and a space-charge ionization detector sensitive to a few ions per second. Multiphoton transitions have been observed to occur both through intermediate atomic states and through intermediate continuum states of the rubidium molecule. In the former case two-photon transitions have been observed from the 52S5^{2}S52S ground state of atomic rubidium to higher-lying n2Dn^{2}Dn2D levels for values of nnn ranging from 9 to 34 and to n2Sn^{2}Sn2S levels for values of nnn from 11 through 20. The fine-structure intervals of the n2Dn^{2}Dn2D levels for n=9toc13n=9 \mathrm{to}c 13n=9toc13 were measured together with the line-strength ratios and were found to be in good agreement with the predictions of a simple theoretical model. At the shorter wavelengths hybrid two-photon resonances were observed to be excited through resonant intermediate continuum states of Rb2{\mathrm{Rb}}_{2}Rb2​. As a result the dispersion curve for two-photon absorption in rubidium showed what appears to be resonant intermediate $p\ensuremath{\pi}(^{3}\ensuremath{\Sigma}_{u1})$ and 0g+{0}_{g}^{+}0g+​ terms dissociating to give a 5P325{P}_{\frac{3}{2}}5P23​​ atom and resulting in the strong development of features corresponding to the $5^{2}P_{\frac{3}{2}}\ensuremath{\rightarrow}n^{2}D_{\frac{3}{2},\frac{5}{2}}$ part of the diffuse series, for $n\ensuremath{\le}50$ in absorption and the $5^{2}P_{\frac{3}{2}}\ensuremath{\rightarrow}n^{2}S_{\frac{1}{2}}$ part of the sharp series. Components to 322D32^{2}D322D and 302S30^{2}S302S were recorded to a precision of 0.3 ${\mathrm{cm}}^{\ensuremath{-}1}$ and quantum defects for these previously unobserved terms were derived. The corresponding hybrid two-photon resonances involving intermediate states dissociating to give a 52P125^{2}P_{\frac{1}{2}}52P21​​ atom were not observed in the wavelength interval available in this experiment.
Singly and doubly charged Ca ions have been produced by multiphoton excitation of Ca vapour with 5 ns, low intensity (⩽3 × 10 11 W cm −2 ) dye-laser pulses in the 675–685 nm wavelength range, including the four-photon 4s 2 1 S 0 → 4p 2 1 S 0 excitation. The intensity and wavelength dependence of the ion yields was recorded as well as the fluorescence emission from excited states of the Ca ion in an effort to identify the excitation pathways leading to single and double ionization. Unambiguous evidence for the absorption of at least two photons above the first ionization threshold was recorded, in agreement with earlier results for Mg and Sr obtained under similar conditions. However, certain characteristics of the process differ significantly from those of the earlier results, despite the apparent similarity in both the atomic structure and the excitation scheme. The most striking and unexpected finding is that for a certain wavelength, the Ca 2+ yield is observable well before the saturation intensity of Ca + and, moreover, it grows with intensity and saturates in parallel with the Ca + yield. Possible mechanisms behind this outcome are discussed in detail as well as their implications for the multiphoton multiple ionization of complex atoms. Our tentative conclusion is that the occurrence of doubly charged ion production before the singly charged ion saturation should not be considered as 'synonymous' with direct (or non-sequential) multiphoton double ionization.
An investigation of the resonant interaction of the rubidium atoms with an intensity (10 kWcm-2 ≤ I ≤ 2 MWcm-2) and a wavelength close to that of the D1 and D2 transitions of the rubidium atom (5S1/2 → 5P3/2 or 5S1/2 → 5P1/2, λD1 = 780 nm, λD2 = 795 nm), which has passes through rubidium vapor with density (1011 - 1014 cm-3) been studied theoretically. The system of equations describing the processes of Collisional ionization and multiphoton ionization of rubidium vapour resonantly excited with nanosecond pulsed laser is solved. The dependence of the ion density on the laser intensity and the atomic density of rubidium are considered. The result of calculations revealed that, both quadratic ion density dependence on laser intensity and linear behaviour of the ion density versus rubidium density for 5S1/2 → 5P3/2 transition is due to photoioization process. In contrast, for 5S1/2 → 5P1/2 transition, the ion density dependence is nonlinear and indicates that the collisional processes play the major contribution in the total ionization. Also, the obtained results showed reasonable agreement with the experimentally measured values of the ion density dependence given by Bakhramov et al. In addition, the analysis of mutual competition between the different ionization processes considered for the ion yield as a function of both laser intensity and atoms density are also presented this work.
The non linear interaction between an intense laser radiation and atoms leads to ionization through the absorption of N photons from the laser radiation via laser-induced virtual states. The multiphoton ionization rate varies as a function of the laser intensity I as IN. We discuss the two most important effects which govern multiphoton ionization processes : resonance effects and laser-coherence effects. In a moderate laser intensity range (107 - 109 W cm-2) corresponding to the two, three or four-photon ionization of atoms, resonance effects play a dominant role while the photon statistics of the laser radiation are relatively unimportant. On the contrary, in the very high intensity range (1012 - 1013 W cm-2) required to observe large Nth - order ionization processes, coherence effects play a dominant role through N! enhancement in the N-photon ionization rate, while resonance effects are completely damped due to the high laser intensity. We conclude by reviewing the possible applications of multiphoton absorption processes in other fields.