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Physical Review A

Two-photon evanescent-wave spectroscopy of alkali-metal atoms

Vladimir G Bordo, Horst‐Günter Rubahn

Published Aug 1, 1999• 19 citations
Publisher

Abstract

The two-photon spectrum of sodium atoms, excited by two counterpropagating evanescent waves, is investigated both experimentally and theoretically. Sub-Doppler linewidths are observed, which are quantitatively reproduced by a rigorous theoretical approach that takes into account optical pumping and transit time broadening due to the translational motion of the arriving and departing atoms through the evanescent-wave fields. The velocity distribution of the atoms desorbing from the surface is found to obey a cosine law, which has a significant influence on the observed line shapes.

DOI
10.1103/physreva.60.1538

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The two-photon spectrum of sodium atoms, excited by two counterpropagating evanescent waves, is investigated both experimentally and theoretically. Sub-Doppler linewidths are observed, which are quantitatively reproduced by a rigorous theoretical approach that takes into account optical pumping and transit time broadening due to the translational motion of the arriving and departing atoms through the evanescent-wave fields. The velocity distribution of the atoms desorbing from the surface is found to obey a cosine law, which has a significant influence on the observed line shapes.
Non-intrusive laser-spectroscopical methods for the diagnostics of the gas-surface interaction in the near-field of a dielectric surface have been developed both experimentally and theoretically. The techniques base on either two-photon evanescent wave excitation or combined evanescent-volume wave excitation. Spectra obtained for sodium atoms at a glass-vacuum interface are quantitatively reproduced by a rigorous theoretical approach. In the case of pure evanescent wave excitation the excitation conditions can be chosen such that either the velocity distribution of desorbing atoms is determined or that atom-surface interaction parameters (polarizability of the adsorbed atoms, desorption rate, sticking coefficient) are obtained from the Autler- Townes splitting of the two-photon lines. By the use of combined evanescent-volume wave excitation one is able to distinguish optically between different groups of atoms interacting with the surface and one can extract their two- dimensional velocity distributions. In addition, information is obtained about superelastic scattering of the atoms interacting with the dielectric substrate.
We study the influence of optical pumping on Doppler-broadened alkali-metal-atom DDD line spectra by solving the time-dependent density matrix for an open two-level system. The time-dependent absorption is averaged over the distribution of interaction times obtained from the three-dimensional beam geometry and atomic velocity distribution and over the longitudinal velocity distribution. The optical pumping is significant at much lower intensities than saturation and depends strongly on the intensity, beam radius, vapor cell length, and spontaneous-decay branching ratio. The result is in agreement with our earlier steady-state solution for a wide range of parameters and predicts two interesting line-shape features.
Abstract High-contrast sub-Doppler resonances observed in alkali-metal atomic vapors in the field of counterpropagating bichromatic laser beams are perspective in quantum metrology for designing a miniature optical frequency standard. Until now, these nonlinear resonances have been investigated only experimentally or using numerical calculations. In our opinion, the development of a simplified theoretical model of the observed resonances, which would provide explicit compact analytic expressions describing the line shape of the resonance, would be extremely important for further evolution of the theory. In this study, we perform such theoretical analysis based on the three-level Λ scheme of the atom. We investigate two regimes, viz., the regime of a low-intensity standing wave with close intensities of counterpropagating beams (I1 ≈ I2) and the regime of a probe wave, in which one of the beams has a noticeably lower intensity than that of the oppositely propagating beam (I2 ≪ I1). The resulting analytic expressions make it possible to determine qualitative differences between these regimes and to separate explicitly the contributions from different nonlinear effects to the light field absorption, including the terms responsible for the formation of a high-contrast sub-Doppler peak. The expressions derived here are in qualitative agreement with experimental data obtained earlier.
Delayed photodesorption of Na atoms from large, surface-bound Na clusters is investigated with a novel technique that includes pulsed plasmon excitation and continuous Doppler-free two-photon evanescent wave detection of desorbing atoms. The spatial confinement of the laser beams within the evanescent wave, the Doppler-free nature of the detection mode, and an accurate evaluation of the kinetic energy of the desorbing atoms in terms of a multiphonon time-of-flight distribution allows temporal information on the decay mechanisms within the cluster to be obtained.
Experiments on open transitions of the D 1 line of alkali metals (Cs and Rb isotopes) reveal the dual structure of saturated absorption resonance in the signal of a high-intensity optical wave in the presence of a low-intensity counterpropagating wave. Theoretical analysis shows that the observed shape of the resonance is associated with the openness of the atomic transition as well as with the Doppler effect for atoms in a gas. The results are of general physical significance for nonlinear spectroscopy and can also find application in metrology (frequency and time standards on open transitions).
We present the results of a theoretical investigation of the fluorescence spectrum from the gas of two-level atoms strongly driven by an evanescent wave (EW). The mean time-of-flight of atoms across the EW is supposed to be less than the relaxation times in the gas volume. Assuming the atomic absorption line to be Doppler-broadened we analyze two specific cases: (1) the atoms over the whole Doppler contour are excited by the EW in the adiabatic-following regime and (2) the EW 'burns out the hole' inside the absorption line. In case (1) in addition to the well- known Mollow triplet the line at the atomic transition frequency appears due to the transient behavior of the atoms departing the surface. In case (2) the spectrum has a sub-Doppler structure sensitive to the type of the atom-surface scattering (diffuse, specular or inelastic). In both cases the spectrum depends on the sticking probability and phases of the scattering in the ground and excited states.