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 dependence of the multiphoton absorption probability for an atomic system on the statistical properties of the incident light is investigated. It is shown, by means of
nth-order time-dependent perturbation theory, that the multiphoton absorption probability depends on the
(n,n)th normally ordered correlation functions of the electromagnetic field. For stationary fields, the transition probability per unit time is constant and is directly related to the reduced cross-spectral correlation function of the electromagnetic field. This expression for the transition probability is then analyzed under various conditions of coherence. Explicit calculations are carried out for thermal light and for laser light, and the transition rates are compared when each has a Lorentzian spectrum. In particular, when the width of the final atomic level is much larger than the bandwidth of the field, the transition rate for thermal light is
n! times higher than with laser light of the same mean intensity. The other extreme case, i.e., when the width of the final atomic level is much smaller than the bandwidth of the field, is also considered in detail. An equation for the density operator of the field is derived; this equation governs the change in the statistical properties of the photon system in
n-photon absorption processes. On the basis of this equation, the time-dependent properties of the photon system are then studied and some physical consequences of these equations are discussed. Some numerical solutions relating to the time dependence of the factorial moments in two-photon absorption processes are presented.
Cross correlation refers to the situation in which the fluctuations in the fields of two or more lasers are correlated in some way. Recently, Thomas et al. [ Opt. Lett.6, 298 ( 1981); Phys. Rev. Lett.48, 867 ( 1982)] proposed the generation of cross correlation between two laser fields interacting with a three-level system as a means of reducing noise and went on to exploit this property in the observation of narrow Ramsay fringes. Dalton and Knight [ J. Phy. B15, 3997 ( 1982)] discussed the theoretical aspects of cross correlation and showed that it produced interesting effects in population trapping for example. We have demonstrated that it has significant effects on the optical double-resonance (ODR) spectra [ J. Phys. B17, L389 ( 1984)]. On the other hand, the effects of non-Lorentzian laser line shapes have been shown by various workers to have significant effects on a wide range of phenomena, such as multiphoton ionization, resonance fluorescence, and ODR. In this paper we present a theory of the interactions of lasers whose fluctuations are governed by the phase-diffusion process with atomic systems that includes the effects of cross correlation and non-Lorentzian line shapes. We derive the basic equations (which in general have to be solved numerically) and obtain analytic results in the case in which the line shape is approximately Lorentzian near line center but falls off faster than a Lorentzian in the wings. We believe that this analytic model shows all the essential features of the interplay between cross correlation and non-Lorentzian line shapes. The theory is applied to the ODR experiment. In particular, we find that the asymmetry of the spectra is strongly affected by these two features, and so is the ODR spectral line shape when the saturating laser intensity is close to the threshold for producing two peaks.
A three-level system driven by two coherent fields on two-photon resonance leads to the trapping of population in a superposition of initial and final states which is immune to further photoexcitation, manifesting itself in a narrow coherence minimum in the absorption spectrum. The authors analyse the effects of laser field bandwidths and cross-correlations on these phenomena. They find that the inclusion of laser bandwidths dephases atomic coherences which leads to the destruction of population trapping and of the narrow coherence minimum in the absorption spectrum. When the driving fields are not cross-correlated, the atomic coherences are similarly dephased in both lambda and ladder systems. If, however, the driving fields are critically cross-correlated, two-photon coherences in the lambda system are unaffected by laser fluctuations; trapping and the coherence minimum persist. For the ladder system, on the other hand, the cross-correlation does not restore the atomic coherences involved.
We study the correlation between level populations, absorption and two-photon coherence in closed Λ- and V-shaped three-level systems interacting with two lasers of arbitrary intensity. Whereas it is well known that maximum two-photon coherence leads to population trapping in Λ-shaped three-level systems interacting with two equally detuned lasers, we demonstrate that minimum two-photon coherence, under saturation conditions, can lead to equal populations in all the levels of a Λ- or V-shaped system when the lasers are symmetrically detuned. Moreover we show that steady-state population inversion between one of the upper levels of a V-shaped system and the ground state can occur when either the detunings are asymmetrical or the upper states decay at different rates. It is shown that this population inversion does not lead to stimulated emission into the lasing modes. These effects are also correlated with two-photon coherence and are explained physically by a cross three-photon scattering process involving two laser photons of different frequencies.