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Physical Review A

Probe spectroscopy in an inhomogeneously broadened three-level system saturated by an intense standing wave

Erkki Kyrola, Rainer Salomaa

Published Apr 1, 1981• 18 citations
Publisher

Abstract

We study inhomogeneously broadened three-level atoms ($\ensuremath{\Lambda}$ configuration). Two energy levels are strongly coupled by an intense standing wave. A weak laser field at an adjacent transition is used as a probe. The probe response is calculated by Green's functions involving continued fractions. The general solution is extendable to other three-level configurations as well to other types of multimode saturators. The connection of various approximate solutions to the exact one is discussed. We concentrate on the Doppler-free case where both transitions have nearly equal frequencies. For this we derive a reasonably accurate closed-form solution, the parameter dependencies of which are investigated in detail. In addition to its average changes the dynamics of the saturated transition plays an important role in the steady-state probe response. The spectra show sharp resonances which cannot be explained in terms of traveling wave superposition models. The width of the velocity distribution has a strong effect on the shape of the spectrum---some resonances are smeared away because of incomplete Doppler dephasing. The relaxation processes influence differently the resonances, which facilitates their interpretation.

DOI
10.1103/physreva.23.1874

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Theory of optical heterodyne three-level saturation spectroscopy via collinear non-degenerate four-wave mixing in coupled Doppler-broadened transitions

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We present a theoretical analysis of high-frequency optical heterodyne saturation spectroscopy in Doppler-broadened coupled three-level systems. The saturating beam, which is assumed to be amplitude modulated at frequency δ (double-sideband suppressed carrier amplitude modulation) is resonant for one of the transitions. Through non-degenerate four-wave mixing processes, this modulation is transferred to a probe beam, resonant for the coupled transition. Saturating and probe fields may be either co-propagating or counter-propagating. The lineshape of the probe modulation is analysed via a third-order perturbation expansion of the atomic density matrix with respect to the incident field amplitudes. The resulting signal is integrated over velocities, in the Doppler limit approximation. Both population saturation effects and coherent (Raman-type, or two-photon) processes contribute to the signal. The various contributions appear as Lorentzian-type resonance doublets. We show that, in the absence of relaxation processes (collisional dephasing, or radiative cascades), destructive interferences between population saturation and coherent two-photon processes are responsible for the disappearance of one resonance doublet. Phase-interrupting collisions are thus predicted to lead to the existence of a « pressure-induced extra-resonance » (PIER) doublet, which could yield information on collisional processes in the impact regime. The properties of the predicted PIER doublets are analysed in relation with other types of PIER signals studied in four-wave mixing, and in time-resolved saturation spectroscopy.

Journal de physique•Jan 1, 1986•10 citations
We study inhomogeneously broadened three-level atoms (\ensuremathΛ\ensuremath{\Lambda}\ensuremathΛ configuration). Two energy levels are strongly coupled by an intense standing wave. A weak laser field at an adjacent transition is used as a probe. The probe response is calculated by Green's functions involving continued fractions. The general solution is extendable to other three-level configurations as well to other types of multimode saturators. The connection of various approximate solutions to the exact one is discussed. We concentrate on the Doppler-free case where both transitions have nearly equal frequencies. For this we derive a reasonably accurate closed-form solution, the parameter dependencies of which are investigated in detail. In addition to its average changes the dynamics of the saturated transition plays an important role in the steady-state probe response. The spectra show sharp resonances which cannot be explained in terms of traveling wave superposition models. The width of the velocity distribution has a strong effect on the shape of the spectrum---some resonances are smeared away because of incomplete Doppler dephasing. The relaxation processes influence differently the resonances, which facilitates their interpretation.
The effects of a strong standing wave field on the absorption behaviour of a weak probe field are studied. An absorptive medium is assumed to consist of stationary two-level atoms with arbitrary decay and pumping scheme. The spectrum with a resonant saturator does not exhibit emissive behaviour as in the travelling wave cases. With a detuned saturator the spectrum closely resembles the corresponding three-level spectrum. These features are explained from the standing wave induced spatial selectivity and inhomogeneity. The connections to Doppler-broadened spectra are discussed.
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.
Previous theoretical results on the influence of a laser on the line shape of a coupled transition-laser-induced line narrowing-have been restricted to the case where the laser is detuned from the center of its atomic gain profile or is in the form of a traveling wave. This paper extends those results to include the case where the laser is an intense standing-wave field tunable to the center of its atomic gain profile (conditions for Lamb dip). The effect may be observed either in transmission, by probing the coupled transition with a weak traveling-wave field coaxial with the laser field, or else in spontaneous emission from the coupled transition viewed along the axis of the laser field. It is now well known that for a laser detuned from the center of its atomic gain profile, two narrow Lorentzian resonances of different widths appear superimposed upon the broad background signal at frequencies symmetrically located about the corresponding line center. When the laser is tuned to the center of its gain profile, however, additional fine structure develops. This structure, which is particularly significant when the laser field is intense, may have important applications in highresolution spectroscopy and laser-frequency stabilization. In this paper the laser frequency may be smaller or larger than the frequency of the coupled transition. In the latter case an intense laser introduces additional splitting effects, even when the laser is detuned. Splitting effects due to weakly saturating laser fields are also discussed. The problem is formulated by expanding elements of the ensemble-averaged density matrix in an infinite series of spatial Fourier components. A perturbation technique is employed, valid for a weak probe field and a standing-wave field of arbitrary intensity. One obtains an expression for emission induced by the probe field due to atoms moving with one velocity, written in terms of continued fractions in the general case and with Bessel functions in an important special case. This expression is integrated over the atomic velocity distribution by means of a computer to obtain the total emission due to atoms moving with all velocities. In some cases the integrated expressions may be written in closed algebraic form. A detailed discussions of line shapes and of the physical processes involved is included.
A previously developed diagrammatic method for calculating the nonlinear response of a dilute gas at near resonance with strong classical radiation fields is extended to include velocity-dependent homogeneous and inhomogeneous broadening phenomena. The method is applied to two-level saturated-absorption (Lamb-dip) spectroscopy. Expressions are obtained for the collision-broadened Lamb dip probed by a weak field in the presence of an arbitrarily strong saturating field and are compared to the usual infinite-Doppler-width, weak-saturation expression. We study the effects of velocity and momentum transfer on the line-shape parameters and discuss the effect of phase-changing and strong inelastic collisions on the intensity.
The nonlinear absorption or gain characteristics of an optical-frequency, Doppler-broadened atomic resonance involving levels with closely spaced structure are analyzed. The level structures are assumed to be resolved with respect to their natural widths, but not necessarily with respect to the Doppler width at the optical transition. The radiation field consists of two closely spaced monochromatic frequencies lying within the Doppler width of the resonance. This type of radiation field may be obtained, for example, from a laser operating in two of its Fabry-Perot resonator modes. It is shown that, because of saturation of level populations and double-quantum Raman transitions between levels, appreciable nonlinear coupling takes place between the two fields. This coupling shows a resonance behavior when the frequency separation of the two applied fields becomes equal to the frequency splitting between two of the components which form either level structure. The width of this resonance is determined entirely by the natural widths of these two level components and not by the Doppler width of the optical transition or the natural width of other level components. When such a resonance occurs, the over-all gain or attenuation characteristics of the atomic resonance change drastically. In practice the frequency spacing of the fields may be kept constant while the level structures are tuned, e.g., magnetically. The effects are analyzed for cases of running-wave and standing-wave radiation fields. The use of this effect in precise determination of level structures as well as mode or transition coupling of a gas laser is discussed. Portions of the analysis are applicable to resonances with more general forms of inhomogeneous broadening.
We present a theoretical analysis of high-frequency optical heterodyne saturation spectroscopy in Doppler-broadened coupled three-level systems. The saturating beam, which is assumed to be amplitude modulated at frequency δ (double-sideband suppressed carrier amplitude modulation) is resonant for one of the transitions. Through non-degenerate four-wave mixing processes, this modulation is transferred to a probe beam, resonant for the coupled transition. Saturating and probe fields may be either co-propagating or counter-propagating. The lineshape of the probe modulation is analysed via a third-order perturbation expansion of the atomic density matrix with respect to the incident field amplitudes. The resulting signal is integrated over velocities, in the Doppler limit approximation. Both population saturation effects and coherent (Raman-type, or two-photon) processes contribute to the signal. The various contributions appear as Lorentzian-type resonance doublets. We show that, in the absence of relaxation processes (collisional dephasing, or radiative cascades), destructive interferences between population saturation and coherent two-photon processes are responsible for the disappearance of one resonance doublet. Phase-interrupting collisions are thus predicted to lead to the existence of a « pressure-induced extra-resonance » (PIER) doublet, which could yield information on collisional processes in the impact regime. The properties of the predicted PIER doublets are analysed in relation with other types of PIER signals studied in four-wave mixing, and in time-resolved saturation spectroscopy.