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AIP conference proceedings

Multiphoton ionization of atomic cesium

R. N. Compton, Cornelius E. Klots, John A. D. Stockdale, C. Dewey Cooper

Published Jan 1, 1984• 0 citations
Publisher

Abstract

We describe experimental studies of resonantly enhanced multi‐photon ionization (MPI) of cesium atoms in the presence and absence of an external electric field. In the zero‐field studies, photo‐electron angular distributions for one‐ and two‐photon resonantly enhanced MPI are compared with the theory of Tang and Lambropoulos. Deviations of experiment from theory are attributed to hyperfine coupling effects in the resonant intermediate state. The agreement between theory and experiment is excellent. In the absence of an external electric field, signal due to two‐photon resonant three‐photon ionization of cesium via np states is undetectable. Application of an electric field mixes nearby nd and ns levels, thereby inducing excitation and subsequent ionization. Signal due to two‐photon excitation of ns levels in field‐free experiments is weak due to their small photoionization cross section. An electric field mixes nearby np levels which again allows detectable photo‐ionization signal. For both ns and np states the ‘‘field induced’’ MPI signal increases as the square of the electric field for a given principal quantum number and increases rapidly with n for a given field strength.Finally, we note that the classical two‐photon field‐ionization threshold is lower for the case in which the laser polarization and the electric field are parallel than it is when they are perpendicular.

DOI
10.1063/1.34651

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We describe experimental studies of resonantly enhanced multi‐photon ionization (MPI) of cesium atoms in the presence and absence of an external electric field. In the zero‐field studies, photo‐electron angular distributions for one‐ and two‐photon resonantly enhanced MPI are compared with the theory of Tang and Lambropoulos. Deviations of experiment from theory are attributed to hyperfine coupling effects in the resonant intermediate state. The agreement between theory and experiment is excellent. In the absence of an external electric field, signal due to two‐photon resonant three‐photon ionization of cesium via np states is undetectable. Application of an electric field mixes nearby nd and ns levels, thereby inducing excitation and subsequent ionization. Signal due to two‐photon excitation of ns levels in field‐free experiments is weak due to their small photoionization cross section. An electric field mixes nearby np levels which again allows detectable photo‐ionization signal. For both ns and np states the ‘‘field induced’’ MPI signal increases as the square of the electric field for a given principal quantum number and increases rapidly with n for a given field strength.Finally, we note that the classical two‐photon field‐ionization threshold is lower for the case in which the laser polarization and the electric field are parallel than it is when they are perpendicular.
Multiphoton ionization (MPI) via two-photon resonance with high-lying Rydberg levels is observed on Na and K atoms in modest (12--120 V/cm) dc electric fields. The field-induced MPI signals are manifested to such an extent that the nominally forbidden MPI via two-photon resonance with the np levels is induced at the same signal levels as or more intensely than the allowed MPI via the ns and nd Rydberg levels. The intensity inversion between the allowed and the forbidden MPI signals is observed on the K atoms in the wavelength region where the two-photon energy is very close to the field-ionization limit.
We present both experimental and theoretical studies of resonantly enhanced multiphoton ionization of cesium atoms. Photoelectron angular distributions for two-photon ionization via the one-photon-allowed 7p2P12,327p^{2}P_{\frac{1}{2},\frac{3}{2}}7p2P21​,23​​ and 8p2P12,328p^{2}P_{\frac{1}{2},\frac{3}{2}}8p2P21​,23​​ intermediate states and three-photon ionization via the two-photon-allowed 8d2D52,328d^{2}D_{\frac{5}{2},\frac{3}{2}}8d2D25​,23​​ resonant intermediate states are reported. The photoelectrons are energy analyzed with a spherical-sector electrostatic energy analyzer with an energy resolution of ~ 0.1 eV and angular resolution of ~ \ifmmode\pm\else\textpm\fi{}2\ifmmode^\circ\else\textdegree\fi{}. A straightforward calculation based upon a finestructure scheme gives excellent agreement with the measured angular distributions for the 2P12^{2}P_{\frac{1}{2}}2P21​​ states. The laser pulse duration is comparable to the hyperfine precession period which allows the hyperfine coupling to partially destroy the anisotropy initially produced in the 2P32^{2}P_{\frac{3}{2}}2P23​​ resonant intermediate states. Quantitative calculations including hyperfine coupling take this into account and provide an expression which gives a reasonable fit to the 2P32^{2}P_{\frac{3}{2}}2P23​​ data.
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.
Multiphoton ionization (MPI) of rubidium atoms at both low (atomic beam) and high (heat pipe) densities is studied using a tunable OPO laser. At high Rb densities ionization of the laser excited ns, np, and nd states occurs both through photoionization and collisional ionization. Excitation of the np states is found to be induced by the external electric field at both low and high densities. In addition, np signal is also seen at very low (E→0) fields in the heat pipe, providing evidence for collision mixing as well as field mixing. At low densities, signal for the high np states initially increases with applied field, but soon saturates (i.e. becomes field independent) while the signal for high nd states decreases with increasing field. At low Rb densities strong resonance features are observed in the energy region between the zero field limit (IP) and the field ionization limit. These features, as well as the field ionization threshold, are found to be dependent upon the angle between the laser polarization and the direction of the applied dc field. Evidence for tunneling through the barrier created by the −e2/r−eEr potential is also presented for ns and nd states.
We derive a set of density matrix equations describing laser photo-excitation and ionization of atomic hydrogen in the presence of an external electric field. The equations are relevant as a description of multiphoton ionization of hydrogen (or deuterium) atoms in laser-produced transient plasmas. The laser wavelength is 243 nm, so that the photoionization is resonant with the 2 s 1/2 level. The electric field causes Stark mixing of the 2 s 1/2 level with the 2 p 1/2 and 2 p 3/2 levels. Because the electric field is taken in the same direction as the linear polarization of the laser, only states with equal m j are coupled, and the atom can be described with a four-level density matrix. The laser bandwidth is taken into account by using the stochastic model of a chaotic laser field introduced by Zoller [1]. We present a few calculations of the probabilities for ionization and excitation of a single hydrogen atom as a function of laser intensity and wavelength.