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Journal of Physics B Atomic and Molecular Physics

Atomic fluorescence in a mode-hopping laser field

Henk F. Arnoldus, Gerard Nienhuis

Published Aug 28, 1986• 8 citations
Publisher

Abstract

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.

DOI
10.1088/0022-3700/19/16/004

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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 fluorescence radiation, emitted by a two-level atom in a perturber bath, is considered. The atom is driven by a single-mode laser with a Lorentzian profile, which is brought about by a fluctuating phase. The stochastics of this phase is taken to be the Markovian random-jump process. The authors derive explicit expressions for the atomic density matrix, the temporal photon correlations and the fluorescence spectrum. The results greatly resemble the results for a non-Gaussian diffusive phase, but deviate slightly from the corresponding expressions in the Wiener-Levy limit of the diffusion process.
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.
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.
A systematic method is presented for averaging the integral equations of motion for the atomic density matrix operator and its quantum correlation functions over the fluctuations of Markovian exciting fields with arbitrary bandwidth. The theory takes into account the statistics of the field to all orders. The method is applied to the investigation of resonance fluorescence in the presence of three different Markovian fields: (i) a phase-diffusion field, (ii) a chaotic field, and (iii) a Gaussian-amplitude field. It is shown that in the case of a resonant, intense phase-diffusion field a center line dip develops in the spectrum of resonance fluorescence when the Rabi frequency is approximately equal to the bandwidth of the field. In the case of amplitude fluctuations the sidebands of the on-resonance spectrum tend to reproduce the probability distribution for the amplitude of the exciting field.
We generalize our earlier formalism to treat the effects of both the finite-bandwidth excitations and finite arbitrary detunings, on the fluorescent spectra and second-order intensity correlation functions in optical double resonance. It is assumed that the bandwidth arises from the phase and/or amplitude fluctuations in the fields driving a three-level atom in cascade configuration. Under the conditions that one or both of these fields are intense, secular approximation and the theory of multiplicative stochastic processes are invoked to derive a Markovian master equation for the atomic-density operator averaged over both phase and amplitude. The quantum regression theorem is used to derive analytical expressions for the fluorescent spectra and the second-order intensity correlation functions which explicitly display the effects due to detunings and fluctuations.
The authors review the various models of fluctuating laser fields which have been used in the past for the treatment of resonance fluorescence of a driven two-level atom. A new treatment of this problem in the case of a partially coherent laser field is given. This method extends that of Zoller (1977, 1978) to a large ratio of atomic decay constant to driving field frequency. The method is a kind of multiple time scale method, applied to a stochastic differential equation, and is of interest in its own right. It gives a systematic expansion in powers of the ratio of the atomic decay constant to driving field frequency, and can in principle be computed to arbitrary accuracy. Computations are presented to assess the effect of the high corrections determined.