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Physica Scripta

Lineshapes in laser spectroscopy of three-level systems

M. Allegrini, E. Arimondo

Published Jan 1, 1997• 0 citations
Publisher

Abstract

The lineshapes originated in a magnetic resonance process for atomic alignment are compared to the lineshapes associated to the resonance of coherent population trapping in a three-level system. An approach based on the tensorial components of the atomic density matrix is applied to analyze both resonances and to evidence the strict relations between the lineshapes.

DOI
10.1088/0031-8949/1997/t70/017

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The lineshapes originated in a magnetic resonance process for atomic alignment are compared to the lineshapes associated to the resonance of coherent population trapping in a three-level system. An approach based on the tensorial components of the atomic density matrix is applied to analyze both resonances and to evidence the strict relations between the lineshapes.
We have detected and analyzed narrow, high contrast coherent population trapping resonances, which appear in transmission of the probe monochromatic light beam under action of the counterpropagating two-frequency laser radiation, on example of the nonclosed three level Λ-system formed by spectral components of the Doppler broadened D2 line of cesium atoms (in the cell with the rarefied Cs vapor). These nontrivial resonances are determined directly by the trapped atomic population on the definite lower level of the Λ-system and may be used in atomic frequency standards, sensitive magnetometers and in ultrahigh resolution laser spectroscopy of atoms and molecules.
We show that a characteristic two-photon lineshape asymmetry arises in coherent population trapping (CPT) and three-photon (N) resonances, because both resonances are simultaneously induced by modulation sidebands in the interrogating laser light. The N resonance is a three-photon resonance in which a two-photon Raman excitation is combined with a resonant optical pumping field. This joint CPT and N resonance can be the dominant source of lineshape distortion, with direct relevance for the operation of miniaturized atomic frequency standards. We present the results of both an experimental study and theoretical treatment of the asymmetry of the joint CPT and N resonance under conditions typical to the operation of an N resonance clock.
Lineshapes of three-level resonance Raman scattering and two-level resonance fluorescence, homogeneously broadened by collisions, in the presence of arbitrarily strong coherent radiation, are studied by means of a tetradic (density-matrix) scattering theory. In the case of medium coupling strength V L to the radiation field (where T 2 -1 <or=V L << tau c -1 , with T 2 and tau c being the coherence damping and collision times, respectively) the Mollow lineshape (1977) for resonance fluorescence is rederived, with proper T 2 and population cross-relaxation effects included. In particular it is shown that relaxation through intermediate non-resonant levels can considerably alter the lineshape in resonance fluorescence. In the case of strong coupling (V L >or approximately= tau c -1 ) the collision rates are modified by the applied field (optical collisions). It is shown that, whereas in self attenuation spectra optical collision rates can be obtained only from line intensity or line wing measurements, in resonance scattering these rates are directly obtained from linewidth measurements.
Effects of an intense saturating radiation on a probe lineshape under Doppler broadening are studied in a three-level system when the frequency of the probe light is higher than that of the saturating light. The problem is analysed in the approximation of weak probe field using an ensemble averaged density matrix. An analytical form of the lineshape is obtained for the resonant saturating field of high intensity at which the Rabi nutation frequency is larger than the Doppler width of the probe transition. The linewidth of probe absorption depends on the Doppler width and the frequency ratio of the probe light to the saturating light. The computer calculation is carried out to find the lineshape in detail at a light intensity where the Rabi nutation frequency is comparable to the Doppler width.
The shape of the coherent-population-trapping (CPT) resonances was investigated theoretically and experimentally at different laser powers. The CPT resonances were observed in fluorescence on the degenerate two-level system of the $({F}_{\ensuremath{\varphi}}=2\ensuremath{\rightarrow}{F}_{f}=1)$ transition of the 87Rb^{87}\mathrm{Rb}87Rb D1{D}_{1}D1​ line by means of a Hanle effect configuration in an uncoated vacuum cell. Numerical simulations based on the density matrix formalism, which take into account the high-rank polarization moment (HRPMs) influence and the velocity distribution of the atoms, were used to calculate the shape of the nonlinear magnetic resonances. The comparison of the theoretical and experimental shapes of the CPT resonances demonstrated that the HRPMs influence the shape at all laser excitation powers, and this influence can be used to explain some peculiarities at the center of the CPT resonance shape.
A review of coherent transients is presented in this article. After a brief discussion of single-wave transients (free induction decay, optical nutation, etc...), two-wave transients, i.e. time-resolved saturation spectroscopy, are treated in more detail. It is shown that this technique of combining both frequency-and-time-resolution in laser spectroscopy allows one to study the various quantum-mechanical processes contributing to the lineshape, in particular (i) the interaction between the laser field and the atomic (or molecular) system, and (ii) the dynamics of the relaxation of the system. Applications to the analysis of Raman-type processes in three-level systems, power-broadening and velocity diffuston are given.