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Physical Review A

Non-Markovian stochastic jump processes. II. The case of resonance fluorescence

Abraham G. Kofman, Reuven Zaibel, Alfred M. Levine, Yehiam Prior

Published Jun 1, 1990• 17 citations
Publisher

Abstract

Strong laser fields, when tuned on resonance to an atomic (molecular) transition, give rise to the well-known triplet of resonance fluorescence. The laser field is normally assumed to be strong and monochromatic, even though the spectrum of real lasers is never a \ensuremath{\delta} function. A standard way to treat laser fluctuations has been to assume a well-defined nominal frequency and a randomly fluctuating phase. Recently we introduced the generalized jump model (GJM) for correlated phase fluctuations, where correlated phase jumps are considered, leading to Markovian as well as non-Markovian stochastic behavior. In the GJM, each phase jump may be correlated to the previous jump, and the degree of correlation, the typical jump size, and the mean time between jumps are the three parameters defining the stochastic character of the laser field. In this paper we apply the GJM model to the case of resonance fluorescence from an atom excited by a stochastic field. The ``standard'' Mollow triplet is obtained in the monochromatic limit of small jumps, and several new predictions are made in the different limits of the stochastic parameters. In the small-jump limit, a new ``field effect'' is predicted. The spectral line shape and the triplet separation deviate from the Mollow predictions for a monochromatic field in a substantial way, giving rise to observable differences.In the highly correlated small-jump limit, which is approximated by the Kubo oscillator model, the previous results are corrected to include nonzero line shifts and extended to the case of non-Lorentzian line shapes. In all regions, even input fields of the same line shape (which would be considered identical in the one-parameter linewidth description) give rise to very different output spectra, justifying the more complete stochastic description. Effective relaxation constants ${\mathrm{\ensuremath{\Gamma}}}_{1}^{\mathrm{*}}$ and ${\mathrm{\ensuremath{\Gamma}}}_{2}^{\mathrm{*}}$ that simplify the description of the spectrum are calculated in all appropriate cases, and ${\mathrm{\ensuremath{\Gamma}}}_{1}^{\mathrm{*}}$ is found to equal the input laser linewidth. In addition to predicting the resonance fluorescence spectra, the present analysis provides a way to extract the stochastic parameters from the nonlinear measurement in those cases where the linear characterization of the input field cannot do it. The analytic work is fully supported by extensive numerical simulations.

DOI
10.1103/physreva.41.6454

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Strong laser fields, when tuned on resonance to an atomic (molecular) transition, give rise to the well-known triplet of resonance fluorescence. The laser field is normally assumed to be strong and monochromatic, even though the spectrum of real lasers is never a \ensuremath{\delta} function. A standard way to treat laser fluctuations has been to assume a well-defined nominal frequency and a randomly fluctuating phase. Recently we introduced the generalized jump model (GJM) for correlated phase fluctuations, where correlated phase jumps are considered, leading to Markovian as well as non-Markovian stochastic behavior. In the GJM, each phase jump may be correlated to the previous jump, and the degree of correlation, the typical jump size, and the mean time between jumps are the three parameters defining the stochastic character of the laser field. In this paper we apply the GJM model to the case of resonance fluorescence from an atom excited by a stochastic field. The standard'' Mollow triplet is obtained in the monochromatic limit of small jumps, and several new predictions are made in the different limits of the stochastic parameters. In the small-jump limit, a new field effect'' is predicted. The spectral line shape and the triplet separation deviate from the Mollow predictions for a monochromatic field in a substantial way, giving rise to observable differences.In the highly correlated small-jump limit, which is approximated by the Kubo oscillator model, the previous results are corrected to include nonzero line shifts and extended to the case of non-Lorentzian line shapes. In all regions, even input fields of the same line shape (which would be considered identical in the one-parameter linewidth description) give rise to very different output spectra, justifying the more complete stochastic description. Effective relaxation constants \ensuremathΓ1∗{\mathrm{\ensuremath{\Gamma}}}_{1}^{\mathrm{*}}\ensuremathΓ1∗​ and \ensuremathΓ2∗{\mathrm{\ensuremath{\Gamma}}}_{2}^{\mathrm{*}}\ensuremathΓ2∗​ that simplify the description of the spectrum are calculated in all appropriate cases, and \ensuremathΓ1∗{\mathrm{\ensuremath{\Gamma}}}_{1}^{\mathrm{*}}\ensuremathΓ1∗​ is found to equal the input laser linewidth. In addition to predicting the resonance fluorescence spectra, the present analysis provides a way to extract the stochastic parameters from the nonlinear measurement in those cases where the linear characterization of the input field cannot do it. The analytic work is fully supported by extensive numerical simulations.
A new non Markovian, correlated jump model for phase fluctuations of an electromagnetic field is introduced'. The phase diffusion, generalized telegraph, Burshtein and Brownian-motion-like models are all obtained from this model in the proper limits. The spectrum and correlation functions of the stochastic field are predicted, and detailed lineshapes of the Mollow triplet of resonance fluorescence are given and shown to depend on the field intensity, a purely non Markovian effect. Two different experimental procedures are proposed for the determination of the stochastic parameters of a laser field.
A new non-Markovian, correlated-jump model for phase fluctuations of an electromagnetic field is introduced. The phase-diffusion, generalized telegraph, Burshtein, and Brownian-motion-like models are all obtained from this model in the proper limits. The spectrum and correlation functions of the stochastic field are predicted, and detailed line shapes of the Mollow triplet of resonance fluorescence are given and shown to depend on the field intensity, a purely non-Markovian effect. Two different experimental procedures are proposed for the determination of the stochastic parameters of a laser field.
A non-Markovian model of correlated phase jumps is introduced for phase fluctuations of an electromagnetic field. This generalized jump model (GJM) treats phase jumps of arbitrary size, occurring at random times; but in contrast to previous work, the jumps are allowed to be fully correlated, partially correlated, or uncorrelated. The degree of correlation is defined by a single parameter derived from the theory. The familiar phase-diffusion model, telegraph-noise model, Burshtein model, and Brownian-motion-like model are all obtained from the GJM in the proper limits. The standard way of characterizing the spectrum of a laser has been the assignment of a single parameter---the linewidth. However, in experiments where the details of the fluctuations are important, or where exact line shapes are measured, this single-parameter characterization might be insufficient. This GJM describes most cases by a set of three stochastic parameters: the degree of correlation between the jumps, the characteristic jump size, and the mean time between jumps. In this paper expressions are derived for the correlation function and the spectrum of a stochastic field in terms of these three stochastic parameters. In addition to analytical work, detailed numerical simulations are presented for the various limiting cases of the model, and the agreement between theory and simulation is excellent. Since the stochastic parameters are not a priori known, a procedure is described for extracting the stochastic parameters from measurable quantities such as the field correlation function or spectrum. Since correlated fluctuations are very common in optics (any stabilization feedback procedure involves anticorrelation), the questions of relevance of the present model to problems of current interest in optical communication and nonlinear optics are also discussed.
The authors apply the recently developed theory of multiplicative stochastic correlation functions with Markovian random jumps to the problem of resonance fluorescence from a two-level atom in a strong laser field. The finite bandwidth of a single-mode laser or the appearance of distinct lines in a multimode laser is considered to be brought about by a random mode-switching process. The two-time dipole correlation functions, which determine the spectral distribution of the fluorescence and the temporal correlations between the emitted photons are averaged exactly over the stochastics of the driving field. The authors' explicit expressions only involve single-time averages, which can be easily evaluated for a given probability distribution. These results generalise and modify earlier results. The authors obtain closed expressions, rather than implicit differential equations, which can handle the continuous case as well, and take into account the initial correlations, which always arise when the laser coherence time is finite. They illustrate the dependence on the stochastics of the laser model by comparing the multimode description with the phase-diffusion process and the Lorentz wave, which all give rise to the same laser profile, but to a different fluorescence spectrum.
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.
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.