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Physical Review A

Theory of Saturated-Absorption Line Shapes

S. Haroche, Francis Hartmann

Published Oct 1, 1972• 293 citations
Publisher

Abstract

A general theory of the saturated-absorption phenomenon in a two-level atomic system is developed, in which the phase relationships between the oscillating atomic dipoles as well as the population differences between energy levels are taken into account. The absorbing gaseous medium considered in this theory is subjected to irradiation by a quasi-running-wave composed of a strong pump field and a weak probe field propagating in opposite directions. Some new interesting results, not predicted by the so-called hole-burning or rate-equation model, are obtained. In particular, the probe-field-transmission peak line shape is found to be markedly different from what is expected according to the rate equations. For finite Doppler widths and a strong saturating pump field, absorption of the probe field can even change sign, and amplification of this field can actually occur. All these features are explained by a close inspection of the evolution of each atomic ensemble of given velocity. Detailed comparison with similar phenomena already observed in rf experiments is presented and permits us to clarify the new predicted effects.

DOI
10.1103/physreva.6.1280

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Physical Review A•Jul 1, 1973•48 citations
A general theory of the saturated-absorption phenomenon in a two-level atomic system is developed, in which the phase relationships between the oscillating atomic dipoles as well as the population differences between energy levels are taken into account. The absorbing gaseous medium considered in this theory is subjected to irradiation by a quasi-running-wave composed of a strong pump field and a weak probe field propagating in opposite directions. Some new interesting results, not predicted by the so-called hole-burning or rate-equation model, are obtained. In particular, the probe-field-transmission peak line shape is found to be markedly different from what is expected according to the rate equations. For finite Doppler widths and a strong saturating pump field, absorption of the probe field can even change sign, and amplification of this field can actually occur. All these features are explained by a close inspection of the evolution of each atomic ensemble of given velocity. Detailed comparison with similar phenomena already observed in rf experiments is presented and permits us to clarify the new predicted effects.
A theory of saturation spectroscopy in three-level gas-vapor systems, including collisional effects, is presented. Using a model of collisions in which they are phase interrupting in their effect on level coherences and velocity changing in their effect on level population densities, the authors calculate the absorption profile of a weak probe field on a given transition when an arbitrarily strong pump field acts on a coupled transition. Line shapes are derived for an arbitrary collision kernel describing the velocity-changing collisions, and these line shapes are evaluated for the collision kernel proposed by Keilson and Storer. Various limiting forms for the line shapes are derived and representative line shapes are displayed. Several new features of the line shapes, including collisionally induced increased probe absorption are discussed. The line shapes are seen to reflect the various collisional processes that may occur in atomic or molecular systems.
We consider in this paper the Doppler-broadened absorption by two-level molecules of a gas from a weak traveling electromagnetic plane wave in the presence of an oppositely traveling strong plane wave at the same frequency. Here the absorption spectrum exhibits a dip that broadens and deepens as the gas is increasingly saturated by the strong wave. This saturation effect has been employed in the recent experiments on the fine structure of atomic hydrogen performed by H\"ansch, Shahin, and Schawlow (HSS). The form, linewidth, and strength of saturation dips in the fine-structure lines are studied for experimental parameters appropriate to the hydrogen experiment. In addition, saturation line-shape curves are calculated for experimental situations in which the strengths of the stronger field give rise to stronger or weaker saturation of the gas medium and varying degrees of Doppler broadening exist. The calculation of shape of the saturation dip and absorption curves for a Doppler-broadened gas of two-level atoms is made exactly; in effect, the strong field is treated as arbitrarily strong by avoiding a perturbation-theory treatment in favor of the exact solutions for a driven two-level system. The general behavior found is in accord with intuition and experimental observations by HSS. There is an optimum saturation power which gives a prominent dip and beyond which the dip suffers "power broadening."
We present a theoretical study of phase-conjugate (PC) emission by backward degenerate four-wave mixing (DFWM) processes in a resonant gas medium. In this study, high-intensity (pump) saturation and Doppler broadening are simultaneously taken into account. We develop a general formalism to deal with the saturation effects in the case of a three-level atom (with degenerate frequencies) and obtain analytical expressions of the PC field amplitude (after integration over the velocity distribution) under the following conditions: (1) the probe beam and one of the pump beams have intensities weak enough to be treated at the lowest perturbation order, whereas the other pump intensity is arbitrarily high; (2) the probe crosses the standing pump wave at grazing incidence. It is shown that the saturation induced by the forward pump (copropagating with the probe beam) leads to entirely different behavior of the nonlinear susceptibility from that induced by the backward pump (counterpropagating with the probe beam). This saturation anisotropy is specific to the inhomogeneous broadening of the gas medium, which is also responsible for the frequency splitting experimentally observed in the intensity line shape of the PC emission for large pump intensities. At saturation, this splitting is theoretically shown to be proportional to the Rabi frequency, with a proportionality coefficient critically dependent on the relaxation processes; in the case of a single-relaxation model, the splitting is equal to 1.5 times the Rabi frequency. The PC intensity line shape is demonstrated to be of dispersive origin in the case of backward saturation, whereas for forward saturation, narrow structures are predicted in both real and imaginary parts of the nonlinear susceptibility, also leading to the intensity line-shape splitting. One also finds that the reflectivity of PC mirrors based on resonant DFWM strongly depends on the origin of the saturation. For a saturating forward pump, the PC emission intensity tends toward zero with increasing pump intensities, and it reaches a finite (nonzero) limit in the case of backward saturation. Most of these predictions have been observed experimentally [ BlochD., Phys. Rev. Lett.49, 719 ( 1982)].
We calculate the two-level pump-probe absorption coefficient including both upper-to-lower-level decay and level decays to a still lower lying reservoir level. We carried out calculations of probe absorption profile for arbitrary ratios of natural width and detuning to the Doppler width associated with a given transition. This theory accounts for contributions from all velocity subclasses of atoms, not only those which are Doppler shifted into resonance with the laser field (Doppler limit).1 We observe and explain new line shape features based on dissimilar decays.
We present in this paper a theory of the saturation effects in degenerate four-wave mixing which makes use of the dressed-atom method. We mainly study the case of a Doppler-broadened line, but several results can be applied to the case of nearly degenerate four-wave mixing for a Doppler-free medium. We show that a close relationship does exist between the two problems : the generated beam is mainly created when the detuning between two incident beams is equal to the Rabi frequency. In the degenerate case, this condition is fulfilled by two velocity groups because of the Doppler shift. We analytically calculate the lineshapes for two-level atoms in the case of forward saturation (the intense pump beam propagates in the same direction than the probe beam) and in the case of backward saturation (the intense pump beam and the probe beam propagate in opposite directions). We also study collisional effects and the influence of the intensity of the weak pump beam when perturbation theory can no longer be applied.
A three-dimensional theory for the resonant interaction of electromagnetic waves with a gas of two-level atoms is formulated in terms of macroscopic variables. The theory is utilized to find the steady-state attenuation of a plane wave in the presence of another plane wave running in the opposite direction with different amplitude. Contributions are included from the reflection of the oppositely running wave by an induced standing-wave inhomogeneity in the population inversion of the medium. The resulting attenuation and reflection coefficients are expressed as velocity integrals of continued fractions. Correspondence is made with existing gas-laser theories, yielding the formulation of a high-intensity ring-laser theory. Analytic approximations for the coefficients are presented for the Doppler-limit cases of both waves weak, one wave weak, and negligible reflection (rate-equation approximation). More-general cases have been calculated numerically. The attenuation coefficients exhibit a Lamb-dip feature. The relative depth of the dip increases rapidly with power at low saturation levels, slowly at high saturation, and is greater in the attenuation of the weaker wave. The width of the dip is nonlinearly power broadened. The shape of the dip is very nearly Lorentzian, except for one special case at high power in which the line splits. The propagation equations for the two waves are integrated over long absorption paths. A large resulting attenuation increases the relative size of the dip while decreasing the power broadening.