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Journal of Physics B Atomic and Molecular Physics

AC Stark effect and fluorescence in modulated laser beams. II. Two-photon stepwise excitations

Ragini Saxena, G. S. Agarwal

Published Feb 14, 1980• 21 citations
Publisher

Abstract

For pt.I see ibid., vol.12, no.12, p.1939 (1979). The modulated fluorescence in an optical double resonance experiment, i.e. when an atom interacts with two intense monochromatic laser beams each of which is weakly modulated in amplitude at frequency Omega , is studied in detail. The modulation rate corresponding to the steady-state population of the highest atomic level exhibits resonant structures at the modulation frequencies Omega =0, +or- alpha 0 , +or-2 alpha 0 due to the dynamical Stark splitting of the various energy levels; alpha 0 being related to the Rabi frequencies alpha 1 and alpha 2 associated with the two lasers and the two atomic transitions, by alpha 0 2 = mod alpha 1 mod 2 + mod alpha 2 mod 2 . The peak at Omega =+or- alpha 0 is the most intense and exhibits splitting when the applied fields are detuned from exact resonance with the respective atomic frequencies. Resonances are observed in the modulation rate of the intermediate-level population at the modulation frequencies Omega =0, +or-2 alpha 0 . In the presence of detunings of the applied fields, additional resonant structures occur at Omega =+or- alpha 0 which increase in magnitude with higher detunings and split. Explicit expressions for the positions, widths and weights of these resonant components are obtained analytically for intense, resonant fields. Numerical results for general values of the laser field strengths and the detunings are given.

DOI
10.1088/0022-3700/13/3/008

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Soviet Journal of Quantum Electronics•May 31, 1986•0 citations
For pt.I see ibid., vol.12, no.12, p.1939 (1979). The modulated fluorescence in an optical double resonance experiment, i.e. when an atom interacts with two intense monochromatic laser beams each of which is weakly modulated in amplitude at frequency Omega , is studied in detail. The modulation rate corresponding to the steady-state population of the highest atomic level exhibits resonant structures at the modulation frequencies Omega =0, +or- alpha 0 , +or-2 alpha 0 due to the dynamical Stark splitting of the various energy levels; alpha 0 being related to the Rabi frequencies alpha 1 and alpha 2 associated with the two lasers and the two atomic transitions, by alpha 0 2 = mod alpha 1 mod 2 + mod alpha 2 mod 2 . The peak at Omega =+or- alpha 0 is the most intense and exhibits splitting when the applied fields are detuned from exact resonance with the respective atomic frequencies. Resonances are observed in the modulation rate of the intermediate-level population at the modulation frequencies Omega =0, +or-2 alpha 0 . In the presence of detunings of the applied fields, additional resonant structures occur at Omega =+or- alpha 0 which increase in magnitude with higher detunings and split. Explicit expressions for the positions, widths and weights of these resonant components are obtained analytically for intense, resonant fields. Numerical results for general values of the laser field strengths and the detunings are given.
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.
The phenomenon of resonance fluorescence provides an interesting manifestation of the quantum theory of light and is a “real world” application of the material of the Chapters 8 and 9. In this process, a two-level atom is typically driven by a resonant continuous-wave laser field and the spectral and quantum statistical properties of the fluorescent light emitted by the atom are measured. Experimentally this can be achieved by scattering a laser off a collimated atomic beam such that the directions of the laser beam, atomic beam, and detector axis are mutually perpendicular as shown in Fig. 10.1. If the driving field is monochromatic, then at low excitation intensity the atom absorbs a photon at the excitation frequency and reemits it at the same frequency as a consequence of conservation of energy. The spectral width of the fluorescent light is therefore very narrow. The situation, however, is considerably more complicated when the excitation intensity increases and the Rabi frequency associated with the driving field becomes comparable to, or larger than, the atomic linewidth. At such intensity levels, the Rabi oscillations show up as a modulation of the quantum dipole moment and sidebands start emerging in the spectrum of the emitted radiation. This so-called dynamic Stark splitting is an interesting feature of the atom–field interaction. In addition to that, the fluorescent light exhibits certain nonclassical properties including photon antibunching and squeezing. In this chapter, we develop a theory of resonance fluorescence to explain these phenomena.
The fluorescence emitted by atoms whose excited states have Zeeman structure is studied for the case of excitation by partially coherent optical sources whose amplitudes are weakly modulated at a low frequency $\ensuremath{\Omega}$. The temporal fluctuations in lasers are taken into account exactly by using the phase-diffusion model of the laser. Analytical results for the modulated fluorescence are presented for the case of weak fields. It is shown that the shape of the fluorescent signal is extremely sensitive to the bandwidth of the field; for example, one gets resonances at a Larmor frequency equal to $\mathcal{s}=\frac{\ifmmode\pm\else\textpm\fi{}\ensuremath{\Omega}}{2}(0,\ifmmode\pm\else\textpm\fi{}\ensuremath{\Omega})$ for broadband (monochromatic) fields. Various limiting cases are treated, and in the limit of very broadband fields, results reduce to those of Corney and Series. The fluorescence is studied both as a function of the modulation frequency and as a function of the magnetic field. Numerical studies of the modulated Hanle signals in intense fields reveal resonant structures in the modulation-frequency scan at $\ensuremath{\Omega}=0,\ifmmode\pm\else\textpm\fi{}{\ensuremath{\alpha}}_{0}$, $\ifmmode\pm\else\textpm\fi{}2{\ensuremath{\alpha}}_{0}({\ensuremath{\alpha}}_{0}^{2}={\mathcal{s}}^{2}+2{\ensuremath{\alpha}}^{2})$ due to the dynamical Stark splitting of the various energy levels, with the strength of the resonances depending on the direction of detection.
A dressed-atom approach is generalised for studying several effects which could be observed on an atomic beam interacting with two monochromatic resonant laser beams saturating two atomic transitions sharing a common level, a situation which occurs frequently in stepwise excitation experiments. The problem of the optimisation of the population of the upper state is investigated. Analytical expressions are derived for the positions, the widths and the weights of the various components of the fluorescence and absorption spectra. The results obtained at the limit where one of the two lasers has a much weaker intensity than the other one are interpreted perturbatively by treating to lowest orders the scattering of the weak laser beam by the atom dressed by the intense one.
The interaction of a strong bichromatic field with a two-level atom has been the subject of numerous experimental and theoretical investigations. We performed an experimental study of the Interaction of an intense 100% amplitude-modulated (AM) field with an ensemble of homogeneously broadened two-level atoms. An optically pumped sodium atomic beam is used as the atomic medium. The field is created by interfering two intense frequency-stabilized laser fields. The frequency of one field is held fixed while another field of equal amplitude is scanned in frequency. The beat frequency produced by interfering the two laser fields is equal to twice the modulation frequency of a 100% AM field. We monitor the time-averaged fluorescent intensity of the atoms as the frequency separation between the two fields is varied. A similar experiment was done in the past in the rf regime.1 For the first time, we report the observation of multiple, well-resolved resonances in the absorption spectrum of the field in the optical regime. We present data and theory for several values of detuning between the fixed field and atomic resonance. The experimental results are in good agreement with theory.
The Stark representation of the resonator field and the first order of perturbation theory of the fluorescence field are used to study the fluorescence spectrum of one and two two-level atoms in an ideal resonator as a function of the initial excitation of the system. It is shown that in the absence of resonator photons (nc = 0) the spectrum obtained for initial excitation of one atom consists of two lines located symmetrically relative to the central frequency ωα. In all other cases the spectrum consists of the central harmonic ωα and of ωα ± 2Ω satellites (Ω is the Rabi frequency). The intensity of collective higher harmonics ωα ± 4Ω is low and it falls on increase in the resonator field as I/nc2. The nonlinearity of the interaction Hamiltonian results in parametric amplification of the ωα + 2Ω harmonics and in attenuation of the ωα–2Ω harmonics. In the case of two atoms it is possible to achieve stimulated fluorescence at the harmonics ωα ± 2Ω.