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Journal of Physics B Atomic and Molecular Physics

Raman-type resonances in two-laser multiphoton ionisation

R. Parzyński

Published Jan 14, 1987• 5 citations
Publisher

Abstract

Higher-order multiphoton ionisation enhanced resonantly by Raman-type transitions is studied theoretically. This higher-order process is found to be stronger than the non-resonant lowest-order one by approximately two orders of magnitude. The shape, position, width, height and area of the resonance peaks that appear due to this process are calculated. Qualitative agreement is found between the theory and the experiment of Feldmann et al. (1986).

DOI
10.1088/0022-3700/20/1/011

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Higher-order multiphoton ionisation enhanced resonantly by Raman-type transitions is studied theoretically. This higher-order process is found to be stronger than the non-resonant lowest-order one by approximately two orders of magnitude. The shape, position, width, height and area of the resonance peaks that appear due to this process are calculated. Qualitative agreement is found between the theory and the experiment of Feldmann et al. (1986).
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.
An expression is derived for the amount of two-photon ionisation produced by sub-nanosecond laser pulses under resonance conditions. On this time scale damping effects can be neglected and the ionisation probability becomes proportional to the cube of the pulse duration. A similar prediction for resonance multiphoton processes of higher order leads to a qualitative agreement with recent experimental observations. Finally, it is demonstrated that the same result can be obtained from a simple analysis of a two-step model.
A theoretical procedure is presented for the evaluation of resonant multiphoton ionisation rates for atoms interacting with intense monochromatic lasers. The essence of the procedure is to treat first the strong coupling by solution of the truncated Schrodinger equation to obtain a time-dependent superposition state. This is then used as the lowest order approximation to iterate the full time-dependent Schrodinger equation to obtain the transition amplitude to the continuum. A model-atom study of the time evolution of the ionisation probability is carried out and the approach to rate behaviour in the long-time limit is demonstrated. Ionisation rates are evaluated for a variety of resonant processes in H, Na and Cs involving one or two lasers, as a function of intensities and detunings. Comparison with experiment is still in a fragmentary stage, and some large discrepancies are found to exist.
We have investigated higher order multiphoton Raman resonances with two pulsed optical frequencies. Multiphoton transfer with up to 50 photons is observed with milliwatts of laser power. We demonstrate that the spectral width of the multiphoton resonances can be far below the Fourier transform linewidth of the driving optical pulses. The functional dependence of the transition linewidth on the number of exchanged photons is found to vary with the pulse shape. Our experiment is performed with laser-cooled rubidium atoms confined in a CO2-laser optical dipole trap.
In a recent experiment involving multiphoton ionisation of Xe it was found that the photoelectron spectrum contained peaks which corresponded to absorption of more than the minimum number of photons required ionise. The effective orders of nonlinearity, furthermore, showed a striking uniformity. The authors investigated these effects with a model approximation consisting of a single bound state and m continua. Simple analytic expressions are obtained for the quantity measured in the experiment and the limit m to infinity is obtained. The results show good qualitative agreement with experiment.
Investigates theoretically a new aspect of radiative collisions on two-photon ionisation of colliding atoms of different species A and B. The authors derive the main characteristics of the resonance appearing in the two-photon ionisation cross section of atom B when the laser frequency is tuned on a resonance transition of atom A which cannot itself be ionised by two-photon absorption. Under some realistic conditions and for reasonable values of the light energy density flux F ( approximately 1 MW cm -2 ), the cross section of the process considered varies as F 2/5 while its width varies as F 1/2 . These predictions are in reasonable agreement with a recent observation on the mixture Sr(A)-Cs(B) by Brechignac et al. (1980).