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Journal of Physics B Atomic and Molecular Physics

Theory of resonant and non-resonant three-photon ionisation

W A McClean, S. Swain

Published Mar 14, 1979• 10 citations
Publisher

Abstract

The theory of resonant and non-resonant three-photon ionisation of a multi-level atomic system illuminated by a not too intense source (in a sense which is defined precisely in the text) with a Lorentzian spectrum is presented. The following new results are obtained: (i) the authors find different expressions for the non-resonant ionisation probability under monochromatic and broad band excitation; (ii) in addition to the usual one- and two-photon resonances connecting the ground state to excited states, the resonance which occurs when the photon energy is equal to the difference in energy between two excited states is discussed; and (iii) the triple resonance (that is the resonance occurring when the conditions for a one-photon and two-photon resonance are simultaneously satisfied) is examined.

DOI
10.1088/0022-3700/12/5/017

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For pt.I see ibid., vol.19, p.79 (1986). The authors study the two-photon ionisation of unpolarised target atoms of caesium in their ground state or in one of the two first excited states 6P 1/2 or 6P 3/2 in the non-resonant region. Circularly, linearly and unpolarised light are considered. For each case they give a systematic analysis of generalised transition probabilities, angular distributions and polarisation phenomena. In particular, it is shown that polarised electrons can be obtained even with linearly or unpolarised light.

Journal of Physics B Atomic and Molecular Physics•Jan 14, 1986•3 citations
The theory of resonant and non-resonant three-photon ionisation of a multi-level atomic system illuminated by a not too intense source (in a sense which is defined precisely in the text) with a Lorentzian spectrum is presented. The following new results are obtained: (i) the authors find different expressions for the non-resonant ionisation probability under monochromatic and broad band excitation; (ii) in addition to the usual one- and two-photon resonances connecting the ground state to excited states, the resonance which occurs when the photon energy is equal to the difference in energy between two excited states is discussed; and (iii) the triple resonance (that is the resonance occurring when the conditions for a one-photon and two-photon resonance are simultaneously satisfied) is examined.
A theory of two-photon ionisation of atomic systems is developed incorporating into the treatment details of the laser spectrum. A general expression for the time-integrated two-photon ionisation probability is obtained together with general expressions for the induced shifts and widths of the atomic levels. These expressions are valid near resonance, when in the ordinary perturbation treatment the energy denominators vanish. The general expressions are then evaluated for the special case of a Lorentzian laser spectrum, when simple analytic results are obtained. The treatment is not confined to the two-level atom or the rotating-wave approximation.
For pt.I see ibid., vol. 17, p.4643 (1984). The authors apply the theoretical results obtained in a previous paper in order to study the two-photon resonant ionisation of atomic caesium in the neighbourhood of the fine-structure doublet 7P 1/2 -7P 3/2 when the incident light is right-hand circularly polarised. This formalism allows one to consider these two resonant states on an equal footing and it includes the effects of the infinite summations involved in higher-order perturbation theory. The numerical results show that the two-photon resonant ionisation of caesium takes place through an anticrossing of levels, at least in the intensity range studied. The temporal behaviour of the probability exhibits two distinct temporal regimes: linear for long interaction times and cubic for the shorter ones. The intermediate regime is characterised by quantum beats. At high intensity values, it is found that the induced light shift of the resonances is time dependent. It is also shown that the contribution of the higher-order effects may explain the slight departures between the theoretical and experimental results in the off-resonant two-photon ionisation of atomic caesium.
The author examines some simple models for multiphoton ionisation which can be constructed when the bound-free transition rates are much smaller than the bound-bound transition rates and considers how to proceed when this condition is relaxed. The author identifies a regime where the transition rate is time independent. If the laser has a sufficiently broad linewidth one can use a rate equation approach; this assertion is justified and applied to two-, three- and N-photon ionisation. If the laser is narrow-band, a density matrix method has to be used and the effects of different laser lineshapes are discussed. In three-photon ionisation the role of optical pumping effects is emphasised. Explicit expressions for the multiphoton ionisation probabilities are presented and finally some extensions of the method are briefly discussed.
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.
Perturbation theory of multiphoton ionisation due to a classical electromagnetic field is modified to allow for intermediate resonances with bound states. Complex energies, generally associated with resonances, do not enter into this formalism. For a monochromatic field of frequency u, a constant ionisation rate can then be defined unambiguously and only such continuum states are excited which correspond to the absorption of energy in integral multiples of hu. As an application, differential and total cross sections for the two-photon ionisation of hydrogen, for frequencies below the n = 3 resonance region, are obtained in closed form. Existing data for generalised cross sections, calculated numerically using the complex coordinate method, are in good agreement with the present results. Finally, the mean fractional ionisation resulting from a pulse of finite duration is estimated on the basis of the associated power spectrum. For short pulses, the time dependence of ionisation exhibits a departure from that expected of a time-independent rate.
For pt.I see ibid., vol.19, p.79 (1986). The authors study the two-photon ionisation of unpolarised target atoms of caesium in their ground state or in one of the two first excited states 6P 1/2 or 6P 3/2 in the non-resonant region. Circularly, linearly and unpolarised light are considered. For each case they give a systematic analysis of generalised transition probabilities, angular distributions and polarisation phenomena. In particular, it is shown that polarised electrons can be obtained even with linearly or unpolarised light.