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Journal of Experimental and Theoretical Physics

Ground-state pump-probe spectroscopy

А. И. Пархоменко, Anatolii M. Shalagin

Published Dec 1, 2007• 3 citations
Publisher

Abstract

The absorption/gain spectrum of a weak probe field is theoretically analyzed for an atomic three-level Λ system driven by a strong pump field and perturbed by collisions with buffer-gas atoms. It is assumed that both pump and probe drive the same transition. When the dark state is sufficiently long lived, the probe spectrum exhibits an extremely narrow (possibly subnatural-width) resonance. It is shown that coherence-preserving collisions drastically (both qualitatively and quantitatively) change the probe absorption spectrum even at a low collision frequency, when Dicke narrowing is negligible. Strong coherence effects on the resonance structure at low gas pressures is explained by a change in refractive index due to coherence-preserving collisions for particles in the resonant velocity group.

DOI
10.1134/s1063776107120011

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Conference on Lasers and Electro-Optics•Jan 1, 1986•0 citations
The absorption/gain spectrum of a weak probe field is theoretically analyzed for an atomic three-level Λ system driven by a strong pump field and perturbed by collisions with buffer-gas atoms. It is assumed that both pump and probe drive the same transition. When the dark state is sufficiently long lived, the probe spectrum exhibits an extremely narrow (possibly subnatural-width) resonance. It is shown that coherence-preserving collisions drastically (both qualitatively and quantitatively) change the probe absorption spectrum even at a low collision frequency, when Dicke narrowing is negligible. Strong coherence effects on the resonance structure at low gas pressures is explained by a change in refractive index due to coherence-preserving collisions for particles in the resonant velocity group.
The absorption (amplification) spectrum of a weak probe field by two-level atoms located in a strong resonant laser field and colliding with buffer-gas atoms is analyzed theoretically. The analysis is performed for low collision frequencies compared to the Doppler absorption linewidth (low gas pressure) and with allowance made for an arbitrary change in the phase of the radiation-induced dipole moment at elastic collisions between gas particles. The phase memory effects have been found to lead to a strong qualitative and quantitative transformation of the probe-field spectrum even at rare collisions, when the well-known Dicke manifestation mechanism of the phase memory effects (the removal of Doppler broadening due to the restriction of the spatial particle motion by collisions) is inoperative. The strong influence of the phase memory effects on the spectral resonances at low gas pressures stems from the fact that the phase-conserving collisions change the velocity dependence of the partial refractive index n ( v ) (the refractive index for particles moving with velocity v ).
We investigate theoretically the spectrum of weak probe field absorption by three-level atoms with the Λ configuration of levels in the field of a strong electromagnetic wave acting on an adjacent transition and colliding with buffer gas atoms. Analysis is carried out for the general case of arbitrary collisional relaxation of low-frequency coherence at a transition between two lower levels. It is shown that, in the absence of collisional relaxation of low-frequency coherence, the probe field spectrum always exhibits clearly manifested anisotropy with respect to mutual orientation of wavevectors of the strong and probe radiation (even under small Doppler broadening). It is found that the probe field spectrum may acquire under certain conditions supernarrow resonances with a width proportional to the diffusion coefficient for atoms interacting with radiation. This fact may form the basis for a spectroscopic method for measuring transport frequencies of collisions between absorbing and buffer particles. A large-amplitude supernarrow resonance (with an amplitude much larger than the amplitude of the resonance near the line center), which is observed in the far wing of the absorption line, exhibits collisional narrowing (a nonlinear spectroscopic analog of the Dicke effect) at collision frequencies several orders of magnitude lower that the Doppler linewidth. Simple working equations proposed for describing the probe field spectrum are convenient for experimental data processing.
The spectrum of weak probe field absorption (amplification) by two-level atoms experiencing collisions with buffer gas atoms in a strong resonance laser field is studied theoretically. Analysis is carried out for systems with a weak Doppler broadening under relatively mild constraints on the strong field intensity for the general case of an arbitrary change in the phase of the radiation-induced dipole moment in elastic collisions of gas particles. It is shown that, in spite of uniform broadening of the absorption line, the probe field spectrum exhibits a clearly manifested anisotropy to mutual orientation of the wavevectors of strong and probe radiation. It is found that the width of resonances in the probe field spectrum under definite conditions (that can easily be created in experiments) is proportional to the diffusion coefficient for atoms interacting with radiation. This fact can form the basis of the spectroscopic method for measuring the transport frequencies of collisions between particles absorbing radiation and buffer particles. It is shown that phase memory effects in collisions strongly modify the probe field spectrum both qualitatively and quantitatively. Simple operative formulas proposed for the probe field spectrum are convenient for experimental data processing.
We present the results of an experimental and theoretical study of the gain (or absorption) experienced by a weak probe beam propagating through a sodium vapor in the presence of an intense pump field that is nearly resonant with the 3s → 3p atomic transition. The probe-transmission spectrum includes three distinct features that result from the modification of the atomic-level structure by the ac-Stark effect. Two of these features can lead to amplification of the probe wave. We measured the dependence of the probe spectrum on the detuning of the pump beam from resonance and on the pressure of a helium buffer gas. The experimentally obtained spectra are in good agreement with the predictions of a theoretical model based on the solution of the density-matrix equations of motion for a two-level atom and including the effects of Doppler broadening. The maximum gain measured in these experiments occurs at one of the Rabi sidebands and leads to a 38-fold increase in the intensity of the probe wave. Under some experimental conditions, we also observed two additional resonances, which are due to stimulated Raman scattering involving the sodium ground-state hyperfine levels.
We describe the effect of thermal motion and buffer-gas collisions on a four-level closed NNN system interacting with strong pump(s) and a weak probe. This is the simplest system that experiences electromagnetically induced absorption (EIA) due to transfer of coherence via spontaneous emission from the excited state to the ground state. We investigate the influence of Doppler broadening, velocity-changing collisions (VCC), and phase-changing collisions (PCC) with a buffer gas on the EIA spectrum of optically active atoms. In addition to exact expressions, we present an approximate solution for the probe absorption spectrum, which provides physical insight into the behavior of the EIA peak due to VCC, PCC, and the wave-vector difference between the pump and probe beams. VCC are shown to produce a wide pedestal at the base of the EIA peak, which is scarcely affected by the pump-probe angular deviation, whereas the sharp central EIA peak becomes weaker and broader due to the residual Doppler-Dicke effect. Using diffusionlike equations for the atomic coherences and populations, we construct a spatial-frequency filter for a spatially structured probe beam and show that Ramsey narrowing of the EIA peak is obtained for beams of finite width.
In this paper we present theoretical calculations relating to pump-probe and four-wave mixing spectroscopy. In pump-probe spectroscopy, one measures the absorption profile for the situation when an arbitrary strong pump field drives a given transition and a probe (weak) field drives the same transition. We have studied the influence of level degeneracy and field polarization on pump-probe and four-wave mixing signals. Our results indicate that for some closed systems (no population loss to the reservoir) it is possible to observe resonances that are characterized by the ground state width. Previous calculations indicate that for a nondegenerate system this resonance can appear only for an open system, the so-called "pressure induced resonances.”1 Our result, which contradicts this conclusion, can be understood by noting the fact that there are in general three irreducible tensor2 (in general) contributions to the line shape (K = 0 population, K = 1 orientation, and K = 2 alignment). Thus, even if the system is closed for the population it may still remain open for orientation or alignment; this effect is responsible for the narrow resonance. Specific calculations are presented for J = 1/2 → 1/2 and J = 1→2 transitions.