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Physical Review A

Multiphoton ionization rate with a non-Lorentzian-band-shape laser

J. J. Yeh, Joseph H. Eberly

Published Aug 1, 1981• 53 citations
Publisher

Abstract

A time-independent single-rate theory for multiphoton ionization processes is developed to cover cases with a partially coherent (finite-bandwidth) driving laser. We use the Ornstein-Uhlenbeck fluctuating-phase model to describe the driving field, which has therefore a non-Lorentzian spectrum, and the effective two-level model to represent the atomic system. We present analytic and numerical methods that permit discussion of the effects of non-Lorentzian band-shape laser light, and we give analytically the bandwidth dependence of the rate in the wings of the ionization curve. Our model contains a simple scaling relationship that permits the rate for $N$-photon-resonant ($N+1$)-photon ionization to be obtained directly from the one-photon-resonant two-photon ionization rate. We treat explicitly the cases $N=1$ and $N=2$.

DOI
10.1103/physreva.24.888

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Physical Review A•Nov 1, 1984•1 citation
A time-independent single-rate theory for multiphoton ionization processes is developed to cover cases with a partially coherent (finite-bandwidth) driving laser. We use the Ornstein-Uhlenbeck fluctuating-phase model to describe the driving field, which has therefore a non-Lorentzian spectrum, and the effective two-level model to represent the atomic system. We present analytic and numerical methods that permit discussion of the effects of non-Lorentzian band-shape laser light, and we give analytically the bandwidth dependence of the rate in the wings of the ionization curve. Our model contains a simple scaling relationship that permits the rate for NNN-photon-resonant (N+1N+1N+1)-photon ionization to be obtained directly from the one-photon-resonant two-photon ionization rate. We treat explicitly the cases N=1N=1N=1 and N=2N=2N=2.
According to laser theory the lineshape of a laser broadened by Ornstein-Uhlenbeck phase fluctuations is non-Lorentzian. The equations describing the interaction of such a laser with atomic systems are cast into a form which has the same structure as the density-matrix equations in the absence of fluctuations but with modified detunings, damping parameters and interaction matrix elements. By these means the authors derive substitution rules for taking into account the effect of these non-Lorentzian lineshapes which generalize those already known for Lorentzian lineshapes arising from Wiener-Levy fluctuations. The theory is applied to two-photon ionisation and analytic expressions are obtained for the rate of this process. For the extended two-level model the authors' results agree with those of Yeh and Eberly (1981) in the appropriate limit, but they also consider a more general model which leads to enhanced single-photon ionisation rates.
A treatment is given of two-photon ionization in which particular attention is paid to the influence of the bandwidth of the ionizing light on the ionization rate. The model adopted for the atom is a common one, including two bound levels and a continuum. The model of the laser is general enough to allow short-term temporal fluctuations of amplitude or phase, and these fluctuations give rise to the laser bandwidth. It is found that the fluctuations have the most interesting effects on the ionization rate when the laser coherence time is shorter than the atomic memory time, as could be expected. In addition to laser bandwidth, we consider the influence on the ionization rate of the detuning of the laser from the intermediate-state resonance, the laser power, and the finite lifetime of the intermediate state. Comparisons with related earlier calculations are made and similarities and differences are pointed out.
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.
The effect of amplitude and phase fluctuations on N-photon excitation from N independent lasers is investigated. Each laser is assumed to have a multi-lorentzian line shape. The Fokker-Planck equation is solved to yield atomic density matrix equations which incorporate the fluctuations. Most of the results discussed are for the lowest-order approximation. No enhancement in the Rabi frequency or transition probability appears, but the Stark shift is found to be enhanced by a factor which is independent of the degree of non-linearity of the process. A general expression for the transition probability in the rate equation regime is presented and its characteristic features discussed. The difference between N-photon excitation from N independent lasers and from a single laser is examined.