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Physical Review A

Angular distribution of electrons from two-photon ionization of Ti atoms

S. A. Edelstein, Melissa Lambropoulos, John A. Duncanson, R. Stephen Berry

Published Jun 1, 1974• 32 citations
Publisher

Abstract

Titanium atoms are excited by light from a nitrogen laser from the $a^{3}F_{4}$ state, near the ground state, through the $x^{3}G_{5}$ state, to become $^{4}F$ ions plus free electrons. The angular distribution of photoelectrons from the process gives limits on the ratio of amplitudes for transitions from the intermediate $4p$ orbital to the final continuum $s$ and $d$ channels. The total number of photoelectrons indicates that the total ionization cross section for the $^{3}G_{5}$ state is 1\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}18}$ ${\mathrm{cm}}^{2}$. While the method can, in principle, provide relaxation times for angular momentum reorientation (an application of the methods of perturbed angular correlations in atomic processes), the present measurements have been carried out under conditions in which no relaxation occurs.

DOI
10.1103/physreva.9.2459

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A general theory is developed to treat two-photon ionization through a single intermediate state in which an arbitrary degree of relaxation may occur. The method is set up to probe the parameters governing the relaxation, by determination of the angular distribution of photoelectrons. The method is applied to the ionization of Na atoms, through the 3p2P123p^{2}P_{\frac{1}{2}}3p2P21​​ and 3p2P323p^{2}P_{\frac{3}{2}}3p2P23​​ intermediate states.
Until recently, the nonlinear interaction between light and matter has been restricted to only low photon energies produced by optical lasers. However, about a decade ago, the rise of free-electron laser facilities revolutionized the field of nonlinear light-matter interaction by delivering intense high-energy light pulses. Today, such lasers are used for research in materials science, chemical technology, biophysical science, solid state physics as well as fundamental research. It is the new experimental possibilities provided by free-electron lasers that motivated the work presented in this thesis. Two-photon ionization process is one of the simplest nonlinear interactions in which absorption of two photons by an atom (or a molecule) leads to promoting one of its bound electrons to continuum. This work presents studies of two-photon ionization of neutral atoms. After a brief historical introduction to the topic of nonlinear light-matter interaction, the density matrix describing the state of an atom and a photoelectron following two-photon ionization is derived. In each successive chapter, part of this density matrix is used to obtain characteristic quantities such as total two-photon ionization cross section, photoelectron angular distributions, ion polarization or degree of polarization of fluorescence photon produced by subsequent decay of the photoion. Physical properties of these quantities are studied and intriguing phenomena, such as elliptical dichroism, polarization transfer as well as relativistic and screening effects are investigated.
We theoretically study multiphoton ionization of the Ca atom irradiated by the second (photon energy 3.13.13.1 eV) and third (photon energy 4.65 eV) harmonics of Ti:sapphire laser pulses (photon energy 1.551.551.55 eV). Because of the dense energy level structure the second and third harmonics of a Ti:sapphire laser are nearly single-photon resonant with the 4s4p4s4p4s4p 1Po{}^{1}{P}^{o}1Po and 4s5p4s5p4s5p 1Po{}^{1}{P}^{o}1Po states, respectively. Although two-photon ionization takes place through the near-resonant intermediate states with the same symmetry in both cases, it turns out that there are significant differences between them. The photoelectron energy spectra exhibit the absence or presence of substructures. More interestingly, the photoelectron angular distributions clearly show that the main contribution to the ionization processes by the third harmonic arises from the far-off-resonant 4s4p4s4p4s4p 1Po{}^{1}{P}^{o}1Po state rather than the near-resonant 4s5p4s5p4s5p 1Po{}^{1}{P}^{o}1Po state. These findings can be attributed to the fact that the dipole moment for the 4s24{s}^{2}4s2 ${}^{1}{S}^{e}\ensuremath{-}4s5p$ 1Po{}^{1}{P}^{o}1Po transition is much smaller than that for the 4s24{s}^{2}4s2 ${}^{1}{S}^{e}\ensuremath{-}4s4p$ 1Po{}^{1}{P}^{o}1Po transition.
An experimental and theoretically study is performed of the angular photoelectron distribution for three-photon ionization of Ba atoms through the 2(omega) -excited intermediate state 6p2 (1So) and the auto- ionized state 6p8s(3P1). Rotation of the polarization plane of dye-laser radiation allowed us to investigate the photoelectron angular distribution. Electrons were counted with the help of a time-of-flight electron spectrometer. Employing the density-matrix formalism, expressions have been obtained for angular dependence of the differential ionizations probability. Possible experiments are discussed.
We report measurements of photoelectron angular distributions via electric quadrupole transitions in cesium atoms using multiphoton excitation techniques. Experimental results are presented for the cases of one-photon resonant, two-photon ionization via the 6d 2{\mathrm{}}^{2}2D3/2{D}_{3/2}D3/2​ and 6d 2{\mathrm{}}^{2}2D5/2{D}_{5/2}D5/2​ electric quadrupole transitions and for one-photon resonant, three-photon ionization via the 5d 2{\mathrm{}}^{2}2 D3/2{\mathrm{D}}_{3/2}D3/2​ and 5d 2{\mathrm{}}^{2}2D5/2{D}_{5/2}D5/2​ transitions. The ratios of the total ionization rates for linearly and circularly polarized light have also been measured for the 6d 2{\mathrm{}}^{2}2D3/2{\mathrm{D}}_{3/2}D3/2​ and 6d 2{\mathrm{}}^{2}2D5/2{D}_{5/2}D5/2​ states. A theoretical analysis and detailed comparison with the experimental results are given.