Lorentzian models for laser line shapes lead to qualitatively incorrect results for off-resonance excitation of atoms. This paper is the first attempt to present a theory of the nonperturbative interaction of an atom with a chaotic field (representing multimode laser radiation having strong amplitude fluctuations) with a line shape falling off faster than a Lorentzian. To this end we suggest a stochastic Markovian model for a non-Lorentzian chaotic field. To solve the multiplicative stochastic differential equations describing the atom-field interaction we propose a "marginal characteristic function approach." This not only reproduces our earlier results in a more elegant way and establishes the relationship between approaches used by other authors in a different context, but also provides the simplest possible basis for our present discussion of ac Stark splitting in double optical resonance. While for a chaotic field with a Lorentzian line shape the asymmetry of the two-peaked off-resonance spectrum is reversed for all values of the detuning compared with the monochromatic case, our present model predicts a reversed peak asymmetry only for detunings smaller than a few laser bandwidths in agreement with experiment. The on-resonance spectrum is dominated by the amplitude fluctuations and is only weakly affected by changes of the spectral line shape of the laser.
Lorentzian models for laser line shapes lead to qualitatively incorrect results for off-resonance excitation of atoms. This paper is the first attempt to present a theory of the nonperturbative interaction of an atom with a chaotic field (representing multimode laser radiation having strong amplitude fluctuations) with a line shape falling off faster than a Lorentzian. To this end we suggest a stochastic Markovian model for a non-Lorentzian chaotic field. To solve the multiplicative stochastic differential equations describing the atom-field interaction we propose a "marginal characteristic function approach." This not only reproduces our earlier results in a more elegant way and establishes the relationship between approaches used by other authors in a different context, but also provides the simplest possible basis for our present discussion of ac Stark splitting in double optical resonance. While for a chaotic field with a Lorentzian line shape the asymmetry of the two-peaked off-resonance spectrum is reversed for all values of the detuning compared with the monochromatic case, our present model predicts a reversed peak asymmetry only for detunings smaller than a few laser bandwidths in agreement with experiment. The on-resonance spectrum is dominated by the amplitude fluctuations and is only weakly affected by changes of the spectral line shape of the laser.
The interaction of an atomic system with a laser having phase fluctuations is studied within the phase-diffusion model, with the finite correlation time of the time derivative of the phase taken into account. This finite correlation time introduces a line shape which is Lorentzian near the center and falls off faster than the Lorentzian at its wings. The authors apply this model to calculate the spectrum of double optical resonance for excitation by a laser having this non-Lorentzian line shape. It is observed that the reversed peak asymmetry reverts to normal far off resonance owing to the cutoff of the laser spectrum, in agreement with recent experiments. Numerical results are presented.
A detailed theoretical analysis of ac Stark splitting in double optical resonance and resonance fluorescence by a nonmonochromatic complex chaotic field is presented. It is shown that a one-photon transition undergoes Stark splitting, which is strongly affected by the intensity fluctuations of the chaotic light. On resonance, the lines in the doublet structure of double optical resonance and the sidebands of the triplet structure in resonance fluorescence are broadened by the intensity fluctuations and tend to copy the Rayleigh distribution of the field amplitude. Off resonance, the asymmetry of the doublet in double optical resonance is reversed and a sideband asymmetry appears in resonance fluorescence for finite bandwidth of the incident light. While on resonance the splitting is always reduced, off resonance the intensity fluctuations may lead to an enhancement of the splitting in comparison to phase-diffusing light.
The effect of a cut off of the Lorentzian laser lineshape (as predicted by the phase-diffusion model of ideal laser theory) on the laser-atom interaction is investigated. The damping terms in the averaged density matrix equation of the atom, arising from the finite laser bandwidth are shown to be multiplied by a detuning-dependent cut-off. For detunings of the laser well within the Lorentzian part of the spectrum, the authors recover the previously derived results, while these damping terms are seen to drop out for detuning larger than the cut-off. Within their model, therefore, a laser with a lineshape falling faster than a Lorentzian, and for large detunings, appears monochromatic to the atom. In particular, the authors obtain qualitative agreement with recent experiments in which the reversed peak asymmetry in the doublet of double optical resonance persists only within a certain range of detuning from resonance.
The effects of different laser line shapes on the intensity and spectrum of resonance fluorescence from a two-level atom are investigated. The laser model considered is that of an ideal single-mode laser operating high above threshold, with constant amplitude and undergoing phase-frequency fluctuations analogous to Brownian motion. As the correlation time of the frequency fluctuations increases from zero to infinity, the laser line shape changes from Lorentzian to Gaussian in a continuous way. It is shown that for intermediate and strong fields, the average intensity of fluorescence in the case of a resonant broadband Lorentzian line shape is higher than that in the case of a Gaussian line shape with the same bandwidth and total power. This is in contrast to the weak-field case where the higher peak power of the Gaussian line shape makes it more effective than the Lorentzian line shape. It is also shown that in the case of a nonzero frequency correlation time (non-Lorentzian line shape) the intensity of fluorescence undergoes non-Markovian fluctuations. In relation to the spectrum of resonance fluorescence, it is shown that as the line shape is varied from Lorentzian to Gaussian the following changes take place: In the case of off-resonance excitation, the asymmetry of the spectrum decreases. In the case of resonant excitation, the center-peak to side-peak height ratio for the triplet structure increases. Moreover, the recently predicted center-line dip, which develops in the spectrum in the case of broadband excitation when the Rabi frequency and the bandwidth are nearly equal, becomes increasingly deeper.
The spectral line shape of the four-wave mixing (FWM) signal, induced by broad bandwidth laser fields, is derived in the case of a nonresonant interaction. The laser fields are assumed to have a Lorentzian spectrum arising from Markovian stochastic fluctuations described by the phase-diffusion, chaotic field, and Gaussian-amplitude models. The usual ``phase conjugating'' geometry for FWM is considered where the nonresonant interaction is determined only by the statistics of, and the correlations between, the pump and probe fields. For each one of the four possible correlation states between the three input fields and for each of the three fluctuating field models, the line shape of the FWM signal is calculated and shown to be particularly sensitive to the field statistics.
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.