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Physical Review A

Stochastic fluctuations in four-wave mixing: A unified theory

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

Published Feb 1, 1988• 13 citations
Publisher

Abstract

A unified approach is presented for the treatment of stochastic fluctuations in four-wave-mixing processes, including uncorrelated and fully or partially cross-correlated input laser fields. The theory allows for phase as well as amplitude fluctuations and covers Markovian and non-Markovian (non-Lorentzian) input line shapes. The analogy between laser field fluctuations and molecular dephasing processes is discussed, and several types of fluctuation-induced resonances are considered. Uncorrelated input fields give rise to resonances similar to those described previously by Agarwal, while correlated input fields cause extra resonances of the type presented by us in earlier publications. Partial cross-correlations are treated here for the first time, with predictions for new effects: Oscillations in the intensity of the generated four-wave-mixing signal as a function of the degree of cross-correlation. The conditions for the experimental observation of these effects are discussed.

DOI
10.1103/physreva.37.1248

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

Abraham G. Kofman, Reuven Zaibel, Alfred M. Levine +1 more

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.

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Fluctuation-induced resonances

Yehiam Prior, Peter Stern

Recently1 a detailed analysis was given for the role played by laser phase fluctuations in NL optics. In that work, the existence of new extra resonances induced by stochastic fluctuations was predicted, based on a derivation starting from the phase diffusion model. In this work we present the results of numerical simulations of laser phase fluctuations. The optical Bloch equations are solved numerically for a phase fluctuating laser. A model of a piecewise constant phase jumping at random between all values is treated, and other models are discussed. Molecular collisions are simulated and compared to phase fluctuations. The collisions give rise to the pressure-induced extra resonance (PIER4), while the phase jumps give rise to stochastic fluctuations-induced extra resonance (SFIER). These simulations show clearly that phase fluctuations may be analogous to real collisions and may cause extra resonances, and indeed, the SFIER4 resonance has recently been observed experimentally.2

International Laser Science Conference•Jan 1, 1986•0 citations
A unified approach is presented for the treatment of stochastic fluctuations in four-wave-mixing processes, including uncorrelated and fully or partially cross-correlated input laser fields. The theory allows for phase as well as amplitude fluctuations and covers Markovian and non-Markovian (non-Lorentzian) input line shapes. The analogy between laser field fluctuations and molecular dephasing processes is discussed, and several types of fluctuation-induced resonances are considered. Uncorrelated input fields give rise to resonances similar to those described previously by Agarwal, while correlated input fields cause extra resonances of the type presented by us in earlier publications. Partial cross-correlations are treated here for the first time, with predictions for new effects: Oscillations in the intensity of the generated four-wave-mixing signal as a function of the degree of cross-correlation. The conditions for the experimental observation of these effects are discussed.
The effect of stochastic laser phase fluctuations on nonlinear optical phenomena are investigated within the phase-diffusion model. Averaged equations of motion are derived in the limit of infinitely short correlation times and the results are applied to multiphoton absorption and to four-wave mixing. The effect of the stochastic phase fluctuations is shown to be equivalent to a T2{T}_{2}T2​ dephasing process, and a procedure is described for the inclusion of this equivalence in many nonlinear-optical problems. When a given mode contributes n photons to a multiphoton absorption process, its contribution to the width of the multiphoton transition is n2{n}^{2}n2 times its own stochastic width. When correlated lasers are used as the excitation sources in four-wave-mixing experiments, (new) stochastic-fluctuation-induced extra resonances in four-wave mixing (SFIER4) will be observed, in complete analogy to the extra resonances induced by collisions [pressure-induced extra resonances in form-wave mixing (PIER4)].
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.
The effect of pump fluctuations on various coherent processes that arise in three-level systems interacting with two external fields is examined. Such coherent processes include the forward Hanle effect and various four-wave mixing effects such as the generation of phase-conjugate signals. A general formulation that enables one to calculate the influence of laser linewidth on the coherent signals produced in various directions is presented. Ensemble averages, over laser temporal fluctuations, of various physical quantities, such as atomic polarization, are calculated. The spectrum of polarization fluctuations is shown to consist of several new features which lead to coherent radiation in different directions depending on the resonant frequencies in the polarization fluctuations. The influence of pump linewidth on pressure-induced extra resonance (PIER) is treated in detail. The possibility of producing a laser-fluctuation-induced coherent signal at one of the atomic frequencies is examined. This new signal, which is produced in a direction different from that of the PIER signal, but has the same type of resonant character as PIER, is found to have significantly different pressure dependence than the PIER signal. The results of our numerical computations are qualitatively explained in terms of the convolutions of products of third-order susceptibilities and pump field-correlation functions.
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.
Recently1 a detailed analysis was given for the role played by laser phase fluctuations in NL optics. In that work, the existence of new extra resonances induced by stochastic fluctuations was predicted, based on a derivation starting from the phase diffusion model. In this work we present the results of numerical simulations of laser phase fluctuations. The optical Bloch equations are solved numerically for a phase fluctuating laser. A model of a piecewise constant phase jumping at random between all values is treated, and other models are discussed. Molecular collisions are simulated and compared to phase fluctuations. The collisions give rise to the pressure-induced extra resonance (PIER4), while the phase jumps give rise to stochastic fluctuations-induced extra resonance (SFIER). These simulations show clearly that phase fluctuations may be analogous to real collisions and may cause extra resonances, and indeed, the SFIER4 resonance has recently been observed experimentally.2