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Journal of Physics B Atomic and Molecular Physics

Doppler-free spectroscopy at a glass-vapour interface by saturated selective reflection at near normal incidence

S. Le Boiteux, Pierre Simoneau, Daniel Bloch, M. Ducloy

Published Mar 14, 1987• 22 citations
Publisher

Abstract

Doppler-free spectra of gas phase atoms near a glass-vapour interface are obtained by monitoring the reflection of a probe beam-instead of its transmission-in three-level saturation spectroscopy. Experiments performed on the 3S-3P-4D cascade system of Na have allowed the authors to monitor two-photon-induced saturated dispersion of Na atoms.

DOI
10.1088/0022-3700/20/5/003

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•Sep 22, 2014•0 citations
Doppler-free spectra of gas phase atoms near a glass-vapour interface are obtained by monitoring the reflection of a probe beam-instead of its transmission-in three-level saturation spectroscopy. Experiments performed on the 3S-3P-4D cascade system of Na have allowed the authors to monitor two-photon-induced saturated dispersion of Na atoms.
Up to now, Doppler-free nonlinear spectroscopy has been applied to atoms inside a gas medium (volume spectroscopy). We have extended these methods to atoms in the vicinity of a surface. The basic principle consists of monitoring reflectivity changes produced when a laser beam, incident on a glass–vapor interface, is brought into resonance with an atomic transition. For Doppler-free spectroscopy, two counterpropagating beams are used to operate velocity selection. If these two beams are under normal incidence in the glass—velocity selection perpendicular to the surface—one observes saturated dispersion (selective reflection sensitive to the real index). For incidence angles in the glass (prism) larger than the critical angle (total internal reflection), a standing evanescent wave is produced in the gas (velocity selection along the surface), and saturated absorption is detected. Experimental demonstration was performed on the Na resonance line; high sensitivity (10−4 relative reflectivity change) and spectral resolution as good as 20 MHz were obtained. The main limitation to better resolution comes from the short atomic transit time in the evanescent wave (typical extension ~λ). Relevant applications of these techniques should also concern the diagnostics of optically thick media, as analysis of interaction between gas-phase atoms and the surface, notably atom–wall collisions, and modification of the spontaneous emission characteristics.
We present an experimental study of non-linear selective reflection at a dielectric/Cs vapour interface, in a three-level cascade-up scheme. The non-linear reflection at the D 2 resonance line is monitored in the presence of a resonant irradiation at 621 nm or 658 nm (6 P 3/2 → 8 D 5/2 , 9 S 1/2 ). A novel type of two-photon-induced reflection resonances specifically connected with atoms desorbing from the surface is observed. We demonstrate that these resonances allow one to monitor the atomic-velocity distribution at vapour-solid interfaces.
We present an experimental study of nonlinear selective reflection at a dielectric--Cs-vapor interface, in a three-level cascade-up scheme. The nonlinear reflection at the Cs D2{\mathit{D}}_{2}D2​ resonance line is monitored in the presence of resonant irradiation at 621 nm or 658 nm (6P3/2{\mathit{P}}_{3/2}P3/2​\ensuremath{\rightarrow}8D5/2{\mathit{D}}_{5/2}D5/2​,9S1/2{\mathit{S}}_{1/2}S1/2​). Experimental reflection spectra with either counterpropagating or copropagating light beams are analyzed and compared with the theoretical predictions of F. Schuller et al. [Phys. Rev. A 47, 519 (1993)]. For a blue-detuned pump and copropagating geometry an alternative type of three-level coherent reflection resonances, specifically associated with desorbing atoms, is observed. Also observed is the nonlinear reflection associated with the off-resonant, two-photon dispersion of atoms moving parallel to the window surface. Probe beam saturation is responsible for the appearance of additional resonant features in reflection spectra. Finally we analyze crossover spectral resonances which arise from nondegenerate, four-wave-mixing processes induced by the combined influence of counterpropagating pump and probe beams, and the pump beam being partially reflected by the window.
We study the cascade three-level selective-reflection spectroscopy for normal incidence at a dielectric--atomic-vapor interface in a pump-probe scheme. Taking into account the effects of spatial dispersion arising from deexcitation by collisions with the interface and the transient response of atoms leaving the surface, we evaluate the modification of the probe-field reflection induced by the presence of the pump field in terms of a nonlocal nonlinear susceptibility. The dependence of this susceptibility on the probe frequency for various given pump frequencies is calculated. Sub-Doppler structures in the selective reflection spectrum are obtained and analyzed. Potential applications to the study of the interaction of highly excited atomic states with the surface are indicated.
The conditions of observation of direct two-photon-induced dispersion in three-level reflection spectroscopy at a vapor-dielectric interface are discussed. One shows how pump frequency modulation allows one to discriminate the two-photon singular contribution associated with atoms moving quasiparallel to the dielectric interface, and therefore single out off-resonant Doppler-free two-photon dispersion in selective reflection. A nonperturbative theoretical approach to two-photon reflection is shown to predict a dynamic Stark shift of the two-photon resonance, which has been experimentally observed on the 6S-6P-8S transition of cesium. @S1050-2947~96!06009-X#
When a vapour is confined, the collisions to the confinement wall usually cause a broadening of the transitions. However velocity selective processes and the coherent enhancement of some transient contributions can lead to sub-Doppler contributions because of the confinement. In the optical range, this had been demonstrated for a one-dimensional confinement with micro- or nano-cells of a small thickness. A two-dimensional confinement in a hollow fiber had shown sub-Doppler contributions, but only equivalent to macrosocpic non linear saturated absorption spectroscopy. Here, we describe experiments showing that a thermal vapor confined in a three-dimensional nanostructure can exhibit sub-Doppler features in a linear regime. We perform reflection spectroscopy on a Cs vapour cell whose window is covered with a thin opal film (typically, 10 or 20 layers of ~ 1µm or 400 nm diameter spheres). We demonstrate, both experimentally and through a modeling that the sub-Doppler structures observed for a large range of oblique incidence angles (~ 30-50°) originate from the interstitial regions of the opal, hence corresponding to a three-dimensional submicrometric confinement. We also show that the partially porous nature of the glass spheres allows some LIAD effects. In a different set of experiments, an atomic vapour is confined in glass medium with large size pores (tens of µm) randomly distributed. The effect of scattered light and fluorescence have been distinguished. Also, sub-Doppler features evolving non linearly with the irradiating intensity are observed, originating in a saturated absorption process induced by the backscattered light .