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Physical Review A

Laser line-shape effects in resonance fluorescence

A. T. Georges, S. N. Dixit

Published May 1, 1981• 42 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.23.2580

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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 ${\mathrm{\ensuremath{\Gamma}}}_{1}^{\mathrm{*}}$ 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.

Physical Review A•Jun 1, 1990•17 citations
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.
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.
The effect of the laser linewidth on the resonance fluorescence spectrum of a two-level atom is revisited. The novel spectral features, such as hole-burning and dispersive profiles at line centre of the fluorescence spectrum are predicted when the laser linewidth is much greater than its intensity. The unique features result from quantum interference between different dressed-state transition channels. c # 1999 Elsevier Science B.V. PACS : 42.50.Hz; 32.80.-t Keywords: Resonance fluorescence; Laser linewidth; Quantum interference The study of resonance fluorescence spectra has provided much fundamental insight into the subject of atom1light interactions. It is well known that for weak laser field excitation, the spectrum exhibits a Lorentzian lineshape, whereas it develops into the Mollow triplet for strong field excitation [1]. The latter is a direct signature of stimulated emissions and absorptions of the atom during the time interval for one spontaneous decay. Recently, considera...
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.
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.