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Journal of Physics B Atomic Molecular and Optical Physics

Theoretical calculation of saturated absorption spectra for multi-level atoms

Liam Maguire, Rick van Bijnen, Emine Meşe, Robert E Scholten

Published May 24, 2006• 50 citations
Publisher

Abstract

We have developed a model for calculating saturated absorption spectra for dipole transitions in multi-level atoms. Using a semiclassical density matrix formalism, we derive a set of coupled differential equations for the internal state of the atom in a standing wave light field. The equations are solved using standard integration techniques. The absorption at each laser detuning is found from an average of the absorption for a number of velocities along the laser field, thermally weighted. The method is relatively efficient computationally yet quantitatively predicts important details of saturated absorption spectra including saturation, crossover resonances, merging of absorption lines at high intensity and optical pumping between hyperfine levels. We have measured saturated absorption and fluorescence spectra of 85 Rb, and compare to our computational results for a 36-level model.

DOI
10.1088/0953-4075/39/12/007

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We have developed a model for calculating saturated absorption spectra for dipole transitions in multi-level atoms. Using a semiclassical density matrix formalism, we derive a set of coupled differential equations for the internal state of the atom in a standing wave light field. The equations are solved using standard integration techniques. The absorption at each laser detuning is found from an average of the absorption for a number of velocities along the laser field, thermally weighted. The method is relatively efficient computationally yet quantitatively predicts important details of saturated absorption spectra including saturation, crossover resonances, merging of absorption lines at high intensity and optical pumping between hyperfine levels. We have measured saturated absorption and fluorescence spectra of 85 Rb, and compare to our computational results for a 36-level model.
A theory of saturation spectroscopy is developed which accounts for effects of level degeneracy. The theory can be applied to those situations in which a pump laser field of arbitrary strength and polarization acts between two manifolds of degenerate or nearly degenerate atomic levels, while a probe laser field of arbitrary strength and polarization acts between a coupled manifold of levels. As such, this theory of "three-level" systems could, in principle, include effects arising from level degeneracy, optical pumping, atomic motion, transient laser fields, different polarizations and strengths for pump and probe fields, and atomic transit across the laser fields. The present calculation, however, is limited to a study of optical pumping and field polarization effects for pump fields of arbitrary strength and weak probe fields interacting with a single velocity subclass of atoms. Probe absorption line shapes clearly display the effects of pump-field strength (Rabi splittings), pump-field polarization (positions and number of Rabi-split resonance peaks), pump-field detuning (positions of resonance peaks), and optical pumping (relative strengths of the resonance peaks). The calculation is carried out with the use of an irreducible tensor basis for the atomic density matrix although a standard (mmm-basis) calculation is included in an appendix.
Using a semiclassical density matrix formalism we have calculated the behavior of multilevel atoms interacting with a standing wave field, and show how complex nonlinear phenomena, including multiphoton effects, combine to produce saturation spectra as observed in experiments. We consider both 20-level sodium and 24-level rubidium models, contrasting these with a simple 2-level case. The influence of parameters such as atomic trajectory and the time the atom remains in the beam are shown to have a critical effect on the line shape of these resonances and the emission/absorption processes. Stable oscillations in the excited state populations for both the two-level and multilevel cases are shown to be limit cycles. These limit cycles undergo period doubling as the system evolves into chaos. Finally, using a Monte Carlo treatment, these processes average to produce saturated absorption spectra complete with power and Doppler broadening effects consistent with experiment.
Using a three-level model and semiclassical density matrix formalism, we show that optical pumping influences both line positions and amplitudes in Doppler-broadened alkali-atom D1 and D2 spectra for intensities much lower than the two-level atom saturation intensity. The influence on the D2 spectrum is particularly interesting due to the presence of closed hyperfine transitions unaffected by optical pumping. This effect is of importance for example when lasers are frequency stabilized using linear absorption or when the alkali-atom vapour pressure is determined using absorption measurements.
A theoretical study on double-resonance optical pumping for the transitions $5{S}_{1/2}\text{\ensuremath{-}}5{P}_{3/2}\text{\ensuremath{-}}4{D}_{3/2,5/2}$ of 87Rb^{87}\text{R}\text{b}87Rb atoms is presented. The full-density-matrix equations in the presence the probe and the coupling laser beams for all relevant magnetic sublevels of the hyperfine levels were solved numerically, and the absorption of a probe beam was calculated as a function of the detuning of the coupling beam. The calculated results were compared with experimental data, and they showed an excellent agreement. The results were also compared with the approximate results calculated when the coherence between the ground and the highest excited levels was neglected. We found that the dominant operating mechanism for double-resonance signals was the optical pumping rather than the two-photon coherence, although the latter affected the signals significantly.
A dressed-atom approach to resonance fluorescence in intense laser fields is presented. Simple and general results are derived which include the now well known predictions concerning two-level atoms but are not restricted to such simple cases. The positions of the various components of the fluorescence and absorption spectra are given by the allowed Bohr frequencies of the total system: atom+laser mode (dressed atom). The master equation, describing spontaneous emission from the dressed atom is solved in the limit of high intensities. Simple expressions, taking into account the effect of cascades, are derived for the widths of the components.
We perform saturated absorption spectroscopy on the D2{D}_{2}D2​ line for room temperature rubidium atoms immersed in magnetic fields within the 0.05--0.13 T range. At those medium-high field values the hyperfine structure in the excited state is broken by the Zeeman effect, while in the ground-state hyperfine structure and Zeeman shifts are comparable. The observed spectra are composed by a large number of absorption lines. We identify them as saturated absorptions on two-level systems, on three-level systems in a V\mathsf{V}V configuration, and on four-level systems in an N\mathsf{N}N or double-N\mathsf{N}N configuration where two optical transitions not sharing a common level are coupled by spontaneous emission decays. We analyze the intensity of all those transitions within a unified simple theoretical model. We concentrate our attention on the double-N\mathsf{N}N crossovers signals whose intensity is very large because of the symmetry in the branching ratios of the four levels. We point out that these structures, present in all alkali-metal atoms at medium-high magnetic fields, have interesting properties for electromagnetically induced transparency and slow light applications.