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Physical Review A

Quantum statistical theory of optical-resonance phenomena in fluctuating laser fields

G. S. Agarwal

Published Oct 1, 1978• 211 citations
Publisher

Abstract

A quantum statistical theory of resonant optical phenomena is developed for the case when the fluctuations of the laser, used for exciting transitions, are important. The general equations describing the dynamics of a relaxing two-level atom (TLA) are solved exactly for different types of mean values and the two-time amplitude and intensity correlations. The phase-diffusion model is adopted for laser fluctuations. The exact results are used to analyze the effect of laser fluctuations on a number of optical effects-optical free-induction decay, adiabatic following, the spectrum of the scattered light from a relaxing TLA, the energy-absorption spectrum from a weak field, Hanle resonances, etc. In each case, the laser fluctuations are found to affect in an important way the characteristics of the above optical-resonance phenomena. For example, the spectrum of scattered radiation from a TLA has the usual three-peak structure for fields at resonance and with strengths $\ensuremath{\alpha}$ above the threshold and for $\ensuremath{\alpha}\ensuremath{\gg}{\ensuremath{\gamma}}_{c}$; however, now the peak heights (widths) are in the ratio $3x$ ($\frac{2}{3x}$), $x=\frac{[{\ensuremath{\gamma}}_{c}+\frac{({T}_{1}^{\ensuremath{-}1}+{T}_{2}^{\ensuremath{-}1})}{3}]}{[2{\ensuremath{\gamma}}_{c}+{T}_{2}^{\ensuremath{-}1}]}$, where ${\ensuremath{\gamma}}_{c}^{\ensuremath{-}1}$ is the correlation time for laser phase fluctuations. For ${\ensuremath{\gamma}}_{c}\ensuremath{\gg}\ensuremath{\alpha}$, one gets a single-peak spectrum. The laser field is treated as a second-quantized field with excitation in either a coherent state or a Fock state. The results, obtained by straightforward perturbation theory, but valid for arbitrary values of the relaxation parameters, detuning, and the laser correlation time, are also presented.

DOI
10.1103/physreva.18.1490

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Physical Review•Nov 1, 1968•212 citations
A quantum statistical theory of resonant optical phenomena is developed for the case when the fluctuations of the laser, used for exciting transitions, are important. The general equations describing the dynamics of a relaxing two-level atom (TLA) are solved exactly for different types of mean values and the two-time amplitude and intensity correlations. The phase-diffusion model is adopted for laser fluctuations. The exact results are used to analyze the effect of laser fluctuations on a number of optical effects-optical free-induction decay, adiabatic following, the spectrum of the scattered light from a relaxing TLA, the energy-absorption spectrum from a weak field, Hanle resonances, etc. In each case, the laser fluctuations are found to affect in an important way the characteristics of the above optical-resonance phenomena. For example, the spectrum of scattered radiation from a TLA has the usual three-peak structure for fields at resonance and with strengths \ensuremathα\ensuremath{\alpha}\ensuremathα above the threshold and for \ensuremathα\ensuremath≫\ensuremathγc\ensuremath{\alpha}\ensuremath{\gg}{\ensuremath{\gamma}}_{c}\ensuremathα\ensuremath≫\ensuremathγc​; however, now the peak heights (widths) are in the ratio 3x3x3x (23x\frac{2}{3x}3x2​), x=[\ensuremathγc+(T1\ensuremath−1+T2\ensuremath−1)3][2\ensuremathγc+T2\ensuremath−1]x=\frac{[{\ensuremath{\gamma}}_{c}+\frac{({T}_{1}^{\ensuremath{-}1}+{T}_{2}^{\ensuremath{-}1})}{3}]}{[2{\ensuremath{\gamma}}_{c}+{T}_{2}^{\ensuremath{-}1}]}x=[2\ensuremathγc​+T2\ensuremath−1​][\ensuremathγc​+3(T1\ensuremath−1​+T2\ensuremath−1​)​]​, where \ensuremathγc\ensuremath−1{\ensuremath{\gamma}}_{c}^{\ensuremath{-}1}\ensuremathγc\ensuremath−1​ is the correlation time for laser phase fluctuations. For \ensuremathγc\ensuremath≫\ensuremathα{\ensuremath{\gamma}}_{c}\ensuremath{\gg}\ensuremath{\alpha}\ensuremathγc​\ensuremath≫\ensuremathα, one gets a single-peak spectrum. The laser field is treated as a second-quantized field with excitation in either a coherent state or a Fock state. The results, obtained by straightforward perturbation theory, but valid for arbitrary values of the relaxation parameters, detuning, and the laser correlation time, are also presented.
A method of calculation of multiple-time correlation functions of the resonance fluorescence light from a two-level atom driven by a realistic laser field with phase and amplitude fluctuations is developed. Both kinds of fluctuations are assumed to be Gaussian. The phase fluctuations are treated in the phase-diffusion model. The averaging over the amplitude fluctuations can be performed in a closed way when the relative mean-square amplitude fluctuation is small compared with the ratio of the amplitude correlation decay rate to the characteristic atomic relaxation rate. There is no restriction to Markovian amplitude fluctuations. Arbitrary values for the mean Rabi frequency are allowed. Results are presented for the intensity, the intensity correlation function, and the spectrum of the fluorescent light. It is shown that even in the case when the relative strength of the amplitude fluctuations is small, significant effects can occur due to the finite correlation length of the fluctuations. The results for fast amplitude correlation decay correspond to the situation without amplitude fluctuations. When the correlation time of the amplitude fluctuations becomes comparable with the atomic relaxation times, the Rabi oscillations of the intensity and the intensity correlation function are nearly washed out, and non-Lorentzian line shapes for the side peaks in the spectrum are observed. It is found that the ratio of the heights of the central peak to the side peak increases with increasing correlation time.
The effects of amplitude and phase fluctuations of the pump laser on the resonance fluorescence under two-photon resonant excitation are studied. The averaging of the stochastic Bloch equations is carried out within the approximation scheme that has recently been applied to the case of one-photon resonant excitation. In the case of two-photon resonant excitation the stochastic pump field gives rise to multiplicative nonlinear Gaussian fluctuation effects. The phase fluctuations are treated in the phase-diffusion model, and the averaging over the amplitude fluctuations is performed by means of generating-function methods. Both the intensity and the intensity correlation of the fluorescent light are studied. When the amplitude fluctuations are weak, the cases of one- and two-photon resonant excitations are similar. The difference between both cases consists of a modification of the Rabi frequency and a faster damping of the Rabi oscillations in the two-photon case. For sufficiently fast correlation decay of the amplitude fluctuations their effect can simply be described by a rate. In the general case of n-photon resonant excitation this rate is larger by a factor of n2{n}^{2}n2 than that in the case of one-photon resonant excitation. When the amplitude fluctuations are sufficiently strong, the Rabi oscillations are ``washed out.'' In the case of one-photon resonant excitation both the intensity and the intensity correlation function of the scattered light develop into step functions over time. In the two-photon case the dynamics of both quantities is determined by a new time constant which acts as both the oscillation time and the damping time. Consequently an overshoot peak occurs in both the intensity and the intensity correlation instead of the tendency to become step functions.
We present a theoretical study of strong laser-atom interactions, when the laser field parameters are subjected to random processes. The atom is modelled by a two- and a three-level system, while the statistical fluctuations of the laser field are described by a pre-Gaussian model. The interaction of the laser-target is treated nonperturbatively by using the calculation method based on the Hermitian Floquet theory. Our aim consists in studying the kinetics of atomic relaxation induced by laser noise. In the resonant case with electric field strengths small with respect to the atomic unit electric strength, the present nonperturbative results are in agreement with those obtained within the rotating wave approximation of Eberly et al and Wodkiewicz et al for an atom modelled by a two-level system. We discuss some examples which demonstrate the destruction of atomic coherence by the noise, the regime of relaxation to the equilibrium state and the optical analogue of motional narrowing. We also give new results for two- and three-level systems, and for a strong laser field at exact resonance, in the case of phase, amplitude noises. The case of fluctuation due to collisions is also discussed. Our numerical results indicate that ionization effects, in the presence of laser noise, can lead to important modifications of the populations for strong laser-atom interactions. The changes in the ionization rates generated by the noise are also investigated.
A quantum-statistical theory of optical Hanle effect is developed for arbitrary intensities and bandwidths of the pump field. The excited- and ground-state level shifts, caused by another light field with appropriate polarization, are directly included in the theory by using the method of time averaging. The laser fluctuations are taken into account exactly by using the phase-diffusion model of the pump laser. The analytical and numerical results for the fluorescence signals are presented for a variety of excitations. Our results in the limiting case reduce to those of Kaftandjian, Klein, and Hanle. Finally, the case of a very broadband excitation under saturation conditions is analyzed and the results for signals in various directions and the polarizations are obtained.
A theory of atomic transitions in correlated stochastic laser fields is developed for the case in which one pulse is assumed to be arbitrarily strong (beyond the fast fluctuation expansion), while the second, time-delayed, pulse is treated in perturbation theory. The statistics of the driving laser field is assumed to be that of a Markov process. We illustrate the technique by calculating the absorption spectrum of a two-level atom in a pump field and cross-correlated probe laser where the field statistics is described by the phase diffusion model.
The probability of an atom undergoing a transition to a given final state by means of two-photon absorption is expressed for arbitrary field states in terms of the second-order normally-ordered field correlation function, evaluated at the position of the atom. In the case of stationary fields, an expression for the absorption rate is found which reduces to a particularly simple form for narrow-bandwidth fields near resonance. The effect of field statistics is illustrated by comparing the absorption rate w2(ch)w_{2}^{}{}_{}{}^{(\mathrm{ch})}w2​​(ch) for chaotic or Gaussian light to the rate w2(l)w_{2}^{}{}_{}{}^{(l)}w2​​(l) for laser light. The rate for laser light is calculated within the context of a particular model based on the assumption of fixed field amplitude and random frequency modulation, and the chaotic light to which it is compared is assumed to have the same (Lorentzian) power spectrum. When the width ${\ensuremath{\kappa}}_{f}$ of the final atomic level is much greater than the bandwidth bbb of the field, we obtain the previously derived result w2(ch)w2(l)=2\frac{w_{2}^{}{}_{}{}^{(\mathrm{ch})}}{w_{2}^{}{}_{}{}^{(l)}}=2w2​​(l)w2​​(ch)​=2. When ${\ensuremath{\kappa}}_{f}\ensuremath{\ll}b$, on the other hand, the ratio between the two rates depends on the (mean) frequency of the field, and assumes the (maximum) value 4 when the field is exactly on resonance.