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Journal of Physics B Atomic and Molecular Physics

Time-dependent spectrum of resonance fluorescence

Joseph H. Eberly, C. V. Kunasz, K. Wódkiewicz

Published Jan 28, 1980• 102 citations
Publisher

Abstract

Attention is focused on the dynamic evolution of the emission spectrum following abrupt excitation of a near-resonant two-level absorber by a strong laser field. The multiphoton character of the absorption-emission process is evident in the AC Stark splitting of the spectrum, which begins approximately half an atomic lifetime after excitation, if the laser field is strong enough. Analytic expressions for the spectra are given of arbitrary laser field strength, atomic lifetime, laser-atom detuning, and the bandwidth of the spectrometer used to analyse the spectrum. Selected graphs are included to illustrate various time-dependent features of the spectrum. The influence on the transient spectrum of three different states of atomic excitation prior to laser irradiation and the effect on the spectrum of irradiation by a phase-noisy laser are also considered. Comparison of the transient spectra from atoms initially prepared in ' pi /2' and '3 pi /2' states show clearly that phase relationships between the irradiating field and the emitting dipole are important even in fluorescence.

DOI
10.1088/0022-3700/13/2/011

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Physical Review A•Apr 1, 1989•12 citations
Attention is focused on the dynamic evolution of the emission spectrum following abrupt excitation of a near-resonant two-level absorber by a strong laser field. The multiphoton character of the absorption-emission process is evident in the AC Stark splitting of the spectrum, which begins approximately half an atomic lifetime after excitation, if the laser field is strong enough. Analytic expressions for the spectra are given of arbitrary laser field strength, atomic lifetime, laser-atom detuning, and the bandwidth of the spectrometer used to analyse the spectrum. Selected graphs are included to illustrate various time-dependent features of the spectrum. The influence on the transient spectrum of three different states of atomic excitation prior to laser irradiation and the effect on the spectrum of irradiation by a phase-noisy laser are also considered. Comparison of the transient spectra from atoms initially prepared in ' pi /2' and '3 pi /2' states show clearly that phase relationships between the irradiating field and the emitting dipole are important even in fluorescence.
The influence of relaxation parameters, as well as temporal fluctuations in the laser field on the modulation rate and phaseshift of the fluorescence from a two-level atom excited by a weakly modulated source is studied in detail. It is shown that, for intense resonant laser fields, the resonance in the modulation rate occurs at the modulation frequency Omega =2 due to the dynamical Stark splitting and has a width equal to 1 / 2 (T 1 -1 +T 2 -1 ). When temporal fluctuations of the exciting laser field are taken into account, the phaseshift of the scattered light is found to be strongly dependent on the bandwidth of the exciting source, as well as the frequency of modulation; hence experimental results on the determination of the lifetime by the phaseshift method have to be interpreted carefully. Numerical results for the modulation rates and phaseshift at different field strengths and various values of T 1 -1 , T 2 -1 , Delta laser bandwidth and Doppler broadening are presented.
We study the transient fluorescence spectra of two-level atoms driven by a strong optical field when the atoms are initially prepared in pure dressed states of the atom-field Hamiltonian. Spectra obtained here differ qualitatively from those observed in the steady state. In the case of steady-state resonant excitation, a three-peaked spectrum symmetric about the laser frequency is obtained; with pure-dressed-state preparation, the symmetry of the spectrum about the driving field is broken---one side peak is initially enhanced and the other is initially suppressed. Furthermore, the temporal oscillations of fluorescence intensity observed in previous calculations of transient fluorescence spectra appropriate to atoms prepared in a superposition of dressed states [J. H. Eberly et al., J. Phys. B 13, 217 (1980)] are suppressed when pure-dressed-state preparation is considered.
A study is presented for the time-dependent resonance-fluorescence spectrum of two-level atoms irradiated by hyperbolic-secant pulsed lasers, allowing for an arbitrary spontaneous-emission rate from the excited level to the ground level. Novel features of the temporally transient spectrum have been observed. The spectrum is dominated by a central peak which oscillates in time and is accompanied by multiple side peaks. Asymptotically (i.e., after the pulse has passed) the side peaks disappear, leaving a tail at the line center which displays a Lorentzian shape of width equal to the sum of the spontaneous-emission rate and the width of the spectrometer considered and of magnitude proportional to the instantaneous intensity of the pulse. The exact behavior of the spectrum is dictated by the area of the engaged pulse and by how the atom is prepared initially. In particular, it is found that the spectrum can be asymmetric even when the laser is tuned to exact resonance if the atoms are initially prepared in a certain class of proper coherent states, irrespective of how the field amplitude may vary in time. An analysis of the spectral symmetry without resorting to any explicit evaluation of the spectrum itself is also presented. Furthermore, the associated optical Bloch equations are solved analytically in terms of hypergeometric functions in a similar manner to that done previously for the undamped two-level Schr\"odinger equation. Specific numerical results are presented for pulses of area equal to \ensuremath{\pi}, 2\ensuremath{\pi}, 3\ensuremath{\pi}, 4\ensuremath{\pi}, and 5\ensuremath{\pi} for both symmetric and asymmetric cases.
The responses of the time-dependent resonance fluorescence spectra of two-level atoms in the presence of (a) strong cw laser fields and (b) short pulsed laser fields to functional disturbances in these fields have been studied by the use of functional-sensitivity-analysis techniques. For the cw case, the transient and steady-state response regions are explored separately. It is found that the response to the field disturbance occurring during the earlier transient period is most prominent at the positions of the well-known three peaks of the corresponding spectrum. In contrast, the response to a disturbance taking place in or near the steady-state region tends to increase the separation between the peaks and lower the intensity of the line center, in exact agreement with the direct calculation of the perturbed spectrum. For the pulsed case, the response to the disturbance is most visible at the line center and at the accompanying multiple peaks caused by the population oscillation of the upper atomic level. The response strongly depends on the magnitude of the pulse area, thus giving rise to distinct asymptotic behavior for (2n+1)\ensuremath{\pi} and 2n\ensuremath{\pi} pulses. As the pulse area becomes large enough to cause significant population oscillation of the upper atomic level, the response of the spectrum shows a resemblance to that of the cw case.
Time-dependent features of the fluorescence radiation from a strongly driven three-level atom in a Raman configuration are studied applying the Eberly-W\'odkiewicz counting-rate definition of the spectrum. Using our earlier formalism, where we assume that one or both of the driving fields are intense, we obtain analytical expressions for the time-dependent fluorescence spectra. We have also studied the influence on the transient spectrum of the initial preparation of the atom in three different dressed states.