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Journal of Physics B Atomic and Molecular Physics

The photoelectron energy distribution in two-photon ionisation

R I Jackson, D P O'Brien, S. Swain

Published Oct 14, 1982• 7 citations
Publisher

Abstract

The authors investigate two-photon ionisation using a generalised rate equation technique for a model in which the atom is assumed to have only two bound levels (the ground state and an excited state) together with a simple continuum of ionised states. Spontaneous emission is allowed from the excited to the ground state, and the laser is assumed to have a finite bandwidth due to phase diffusion. The photoelectron energy distribution is calculated; it is found that if the Rabi frequency exceeds the ionisation rate the energy spectrum is a sensitive function of the linewidth and spontaneous emission rate, whereas if the ionisation rate exceeds the Rabi frequency then the sensitivity of the energy spectrum to these parameters depends upon the initial state of the system. A quite small value of laser linewidth is found to considerably reduce the heights of peaks and increase the widths. Analytic and numerical results are presented.

DOI
10.1088/0022-3700/15/19/009

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The authors investigate two-photon ionisation using a generalised rate equation technique for a model in which the atom is assumed to have only two bound levels (the ground state and an excited state) together with a simple continuum of ionised states. Spontaneous emission is allowed from the excited to the ground state, and the laser is assumed to have a finite bandwidth due to phase diffusion. The photoelectron energy distribution is calculated; it is found that if the Rabi frequency exceeds the ionisation rate the energy spectrum is a sensitive function of the linewidth and spontaneous emission rate, whereas if the ionisation rate exceeds the Rabi frequency then the sensitivity of the energy spectrum to these parameters depends upon the initial state of the system. A quite small value of laser linewidth is found to considerably reduce the heights of peaks and increase the widths. Analytic and numerical results are presented.
The authors study the resonance lineshape in two-photon ionisation of atoms when the power broadening due to the bound-bound transitions is by far the dominant broadening mechanism. The authors consider the effect on the lineshape of turn-on of the laser-atom interaction, spontaneous emission and laser linewidth, and show that several different types of lineshapes can result depending on the conditions involved. The authors also consider the photoelectron spectrum, and show that it is also sensitive to these same parameters.
The authors treat a model for photoionisation in which the atom has many bound atomic levels and the laser may be either monochromatic or possess a finite bandwidth. The treatment is restricted to the case where the laser is not sufficiently intense to cause Stark splitting of the atomic energy levels. They obtain an expression for the two-photon ionisation probability as a function of time which covers both resonant and non-resonant excitation. They identify several time regimes where the probability takes on a particularly simple form. In particular they discuss the short time behaviour and the conditions under which a time-independent transition rate exists. Numerical plots of the ionisation probability against laser frequency for a wide range of pulse durations are given for the two-level model.
Non-perturbative completely analytic calculations of the spin polarisation of photoelectrons produced in resonant two-photon ionisation of alkali atoms with exciting and ionising light beams are presented. A well justified alkali atom model composed of four discrete states and the continuum is applied. Contrary to simpler models it enabled one to obtain results valid when the effective resonance Rabi frequency exceeds the frequency separation between the two components forming a given fine-structure energy doublet at resonance. It is shown that in this limit the photoelectron polarisation depends critically on whether a light or heavy alkali atom is ionised. In the former case the photoelectron polarisation is proved to be a copy of the electronic polarisation of the atom, whereas in the case of heavier alkalis it departs appreciably from that of the ionised atom due entirely to spin-orbit perturbation of radial wavefunctions of P discrete states. It is also shown how the author's present results go over into those previously obtained for weaker exciting fields.
Atoms in an autoionisation state can be excited to higher states in the continuum as well as performing spontaneous transitions to bound states by laser-induced autoionisation. Both effects are investigated by means of the reaction matrix. Results obtained by Armstrong et al (1978) using the same method are extended. The shape of the photoelectron spectrum is different from that of the photon spectrum emitted from the autoionisation state but is similar to that of the photon spectrum emitted from the same bound state which is excited to the ionisation states in the former case. It is predicted that the shape of the fluorescence yield with the pump laser detuning is Lorentzian. The multiphoton process contributes to the photoelectron spectrum in a complicated way.
A density-matrix formulation is given of two-photon ionisation of alkali atoms, for two incoming light pulses of arbitrary direction, polarisation, pulse duration and time difference. The frequency of one of the pulses coincides with a resonant transition. The emphasis is on separating out angular momentum factors from the basic physics contained in the radial matrix elements of the atomic electric dipole. The bandwidth of the exciting light is assumed large compared to natural and induced linewidths. The polarisation of the photoelectron is calculated with or without saturation of the excitation for various values of the nuclear spin.
Two-laser multiphoton ionisation under the autoionising-like resonance condition is studied theoretically within an extended atomic model dictated by the experiment of Feldmann et al (1986). Ordinary coupling between a selected pair of bound states via the continuum only is supplemented in the author's model by Raman-type coupling involving the atomic spectrum below the ionisation threshold. In the case considered this additional Raman coupling enhances the ionisation rate to a much greater extent than the coupling via the continuum can do. The Raman coupling modifies the autoionising-like shape parameter and is decisive as far as the resonance peak profile is concerned. Exploiting this Raman coupling within the atomic model with four effective bound states, the author gives explanations for all the details of the ionisation spectrum detected by Feldmann et al, i.e. the number of resonance peaks, their strength, fine structure, shape, relative heights and sensitivity to the laser field.