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Journal de physique

Resonant multiphoton ionization of caesium atoms

G. Petite, J. Morellec, Didier Normand

Published Jan 1, 1979• 54 citations
Publisher

Abstract

This paper studies the resonant multiphoton ionization (RMPI) phenomenon, in the case of caesium atoms interacting with the intense field of a neodymium-Glass laser. In the first part, we present a recent theory of RMPI, in a simplified form in order to obtain the main informations on the physics of RMPI. Then we present two experiments of RMPI : four-photon ionization of the caesium atom in its ground state, with a three-photon resonance on the 6F level and three-photon ionization of the caesium atom is its 62P3/2 state with a two-photon resonance on the 12F level. In the first experiment, the internal structure of the resonant transition is resolved, enabling us to point out and analyse the important effect of pulse shapes and focusing conditions on our experimental results, which are discussed in detail. We also give some new interpretations of results published previously [1]. In the second experiment, we measure the 12F fine structure — which is found to be (0.016 ± 0.008) cm-1 — and show that we have reached the limits imposed by the Doppler effect. These experimental results are in good agreement with the theoretical predictions suggesting that the physical picture given of RMPI by recent works on this subject is satisfactory.

DOI
10.1051/jphys:01979004002011500

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Saturation effects in multiphoton ionization

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We have studied two-photon resonant three-photon ionization of atomic sodium vapor. A dye laser tuned to either the 4d or 5s two-photon allowed transition was used to excite the atom and a second more intense laser (λ = 7000 Å) was used for ionization. The ion yield was measured as a function of resonant laser intensity and detuning, the nonresonant laser intensity, and the temporal overlap of the exciting and ionizing laser pulses. We have found1 that at high laser intensities the photoionization yield decreases as the nonresonant laser intensity is increased. When tuned to the 5s level a value of ~−0.6 was obtained for the exponential index even with the resonant laser tuned to maximize the ion yield. A theoretical model including the effects of Stark shift of the ground state, power broadening of the intermediate level due to saturation of the two-photon transition and by rapid transitions to the ionization continuum was used to predict the experimental results. Good agreement between theory and experiment required the use of a photoionization cross section for the 5s level which was ~20 times greater than the accepted value. Results for photoionization from the 4d level are also presented.

Annual Meeting Optical Society of America•Jan 1, 1985•0 citations
This paper studies the resonant multiphoton ionization (RMPI) phenomenon, in the case of caesium atoms interacting with the intense field of a neodymium-Glass laser. In the first part, we present a recent theory of RMPI, in a simplified form in order to obtain the main informations on the physics of RMPI. Then we present two experiments of RMPI : four-photon ionization of the caesium atom in its ground state, with a three-photon resonance on the 6F level and three-photon ionization of the caesium atom is its 62P3/2 state with a two-photon resonance on the 12F level. In the first experiment, the internal structure of the resonant transition is resolved, enabling us to point out and analyse the important effect of pulse shapes and focusing conditions on our experimental results, which are discussed in detail. We also give some new interpretations of results published previously [1]. In the second experiment, we measure the 12F fine structure — which is found to be (0.016 ± 0.008) cm-1 — and show that we have reached the limits imposed by the Doppler effect. These experimental results are in good agreement with the theoretical predictions suggesting that the physical picture given of RMPI by recent works on this subject is satisfactory.
This paper reports the four-photon ionization of caesium atoms when the laser frequency is tuned through the resonant three-photon transition 6S → 6F. This experiment was performed by using a tunable-wavelength bandwidth-limited subnanosecond laser pulse at 1.06 μm, in the 108-109 W.cm-2 laser intensity range. Pulse widths of 1.5 ns, 50 ps, and 15 ps were used. The resonant character of the multiphoton ionization process was observed, even with the shortest pulse of 15 ps. Nevertheless the influence of a temporal effect is demonstrated according to theoretical predictions. The resonance shift ΔE of the 6S → 6F transition energy was found to be linear with the laser intensity I within the range 108-109 W.cm-2. ΔE = α I, with α = 2 cm-1/GW.cm-2. This result confirms previous measurements performed with single-mode 35 ns laser pulses and is in very good agreement with calculated resonance shifts.
Two investigations are reported on the application of resonantly enhanced multiphoton ionization (RMPI) to gaseous mixtures of an atomic vapor and a few Torr of argon. Photon fluxes large enough to ionize atoms by RMPI were produced by focussing down the light from a tunable pulsed dye laser. The irradiances generated were of the order of 500MWcm⁻². Ionization was detected by a voltage biased wire electrode that simply collected the photoelectrons either directly or after some gas multiplication. One investigation was the measurement of the dependence of RMPI processes in mercury on the polarization of the incident light for comparisons with theoretical calculations. The processes were four-photon resonant absorptions to either a ¹S₀ or ¹’³D₂ level followed by single photon ionization. Complete photoionization of all atoms excited to the resonant levels is established and the measured polarization dependences are found to agree with the calculated polarization dependence for the resonant excitation step of the RMPI process. Unexplained observations of the distortions in the polarization dependence of the ion yield and the absorption linewidth of the 6d ¹D₂ resonance are discussed. The second investigation was a study of the density dependent electric dipole forbidden two-photon resonant transition ²S → ²P in three-photon RMPI spectra of the Rydberg states of potassium. Stark interactions are shown to be unlikely and too weak. From the characteristics of the spectra, the excitation process is identified as a laser-assisted collision interaction.
This work reports the multiphoton ionization of cesium atoms, via resonance with the 6F6F6F level, by interaction with a single transverse and longitudinal mode neodymium-glass laser beam. At a low rate of ion production, when the laser frequency is tuned through resonance, the laser intensity necessary to create a constant number of ions passes through a minimum, as expected, for a three-photon energy equal to the unperturbed $6S\ensuremath{\rightarrow}6F$ transition energy. But for a higher ionization rate, involving larger laser intensities, a departure from expectation is observed which is interpreted as a consequence of an energy shift of the transition. The level shifts are demonstrated in another way by their strong effect on the experimental order of nonlinearity of the interaction, Kexpt{K}_{\mathrm{expt}}Kexpt​. A sharp variation of Kexpt{K}_{\mathrm{expt}}Kexpt​ is observed when the energy shift of the $6S\ensuremath{\rightarrow}6F$ transition exactly compensates the wavelength detuning of the laser. The latter method gives shift values which are found to be independent of the large variations of the interaction volume under conditions of resonance. Both methods give a linear dependence of the shifts on the laser intensity. Identification of these shifts with energy shifts of the $6S\ensuremath{\rightarrow}6F$ transition is subject to theoretical reservations and needs further experimentation.
We report resonant multiphoton ionization in neon. The study of the interaction volume shows that the size of the focused region depends on the laser power, order of interaction, and energy of photon. Thus we have chosen a resonant approach. The results show a discrepancy of 6 cm−1 between the experimental multiphoton resonance and the theoretically predicted one. We explain this discrepancy by the perturbative effect of the intense electromagnetic field of the laser on the resonant atomic level 11p [3/2]1,2 of neon.
Experimental and theoretical results are presented for resonantly enhanced three-photon ionization of cesium atoms in the wavelength range from 830 to 950 nm. The accidental near resonance of the 6p2P32,126p^{2}P_{\frac{3}{2},\frac{1}{2}}6p2P23​,21​​ levels at the one-photon energy and the near resonance at the two-photon level with the 6d2D32,526d^{2}D_{\frac{3}{2},\frac{5}{2}}6d2D23​,25​​ states gives rise to large ionization signals and interesting anomalies in the relative intensities of the fine-structure levels. "Hybrid resonances" are observed which involve the production of 6p2P126p ^{2}P_{\frac{1}{2}}6p2P21​​ atoms from molecular cesium. One hybrid resonance involves ionization of the 6p2P126p ^{2}P_{\frac{1}{2}}6p2P21​​ state via an electric quadrupole transition ($6p ^{2}P_{\frac{1}{2}}\ensuremath{-}7p ^{2}P_{\frac{3}{2}}$). Both experimental and theoretical photoelectron angular distributions are compared for all of the observed resonances except for the 6p2P326p ^{2}P_{\frac{3}{2}}6p2P23​​ state where the signals were too weak for such a measurement. Agreement between experiment and theory is fair for three-photon ionization via the 6p2P126p^{2}P_{\frac{1}{2}}6p2P21​​ state. Comparison of experiment and theory for the case of the 6d2D32,526d^{2}D_{\frac{3}{2},\frac{5}{2}}6d2D23​,25​​ states indicates that hyperfine coupling during the laser-pulse duration may be important. The angular distributions for the hybrid resonances show the general behavior predicted by theory but the features appear broadened.
We have studied two-photon resonant three-photon ionization of atomic sodium vapor. A dye laser tuned to either the 4d or 5s two-photon allowed transition was used to excite the atom and a second more intense laser (λ = 7000 Å) was used for ionization. The ion yield was measured as a function of resonant laser intensity and detuning, the nonresonant laser intensity, and the temporal overlap of the exciting and ionizing laser pulses. We have found1 that at high laser intensities the photoionization yield decreases as the nonresonant laser intensity is increased. When tuned to the 5s level a value of ~−0.6 was obtained for the exponential index even with the resonant laser tuned to maximize the ion yield. A theoretical model including the effects of Stark shift of the ground state, power broadening of the intermediate level due to saturation of the two-photon transition and by rapid transitions to the ionization continuum was used to predict the experimental results. Good agreement between theory and experiment required the use of a photoionization cross section for the 5s level which was ~20 times greater than the accepted value. Results for photoionization from the 4d level are also presented.