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Physical Review A

Three-level nonlinear selective reflection at a glass–Cs-vapor interface

Anne Amy‐Klein, Solomon M. Saltiel, O. A. Rabi, M. Ducloy

Published Oct 1, 1995• 13 citations
Publisher

Abstract

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 ${\mathit{D}}_{2}$ resonance line is monitored in the presence of resonant irradiation at 621 nm or 658 nm (6${\mathit{P}}_{3/2}$\ensuremath{\rightarrow}8${\mathit{D}}_{5/2}$,9${\mathit{S}}_{1/2}$). 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.

DOI
10.1103/physreva.52.3101

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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 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 consider nonlinear selective reflection on the interface between dielectric media and dilute vapors of three-level atoms. Assuming a pump-probe scheme with cascade-type excitation, we study the modification \ensuremath{\Delta}R of the reflection coefficient of the probe induced by the presence of the pump. We extend previous calculations of the frequency spectrum of \ensuremath{\Delta}R made for low probe power to the case of arbitrary probe power. One then obtains a strong resonance which has already been observed experimentally. Moreover, for the two-photon resonance present in the low-intensity spectrum, a power splitting can be predicted with increasing intensity \textcopyright{} 1996 The American Physical Society.
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.
We report on recent developments in selective reflection spectroscopy at a vapor interface. In FM linear spectroscopy, the long range van der Waals surface interaction, responsible for lineshapes distortions and shifts, is quantitatively well understood with respect to the nature of the dielectric surface. Pump‐probe saturation effects in reflection spectroscopy on a two‐level system offer alternate ways of probing surface interaction, while nonlinear reflection spectrsocopy on a three‐level cascade system provides a unique tool for probing in a vapor cell the velocity distribution of desorbing atoms.
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#
Selective reflection spectroscopy at an interface with a low-density resonant vapor, especially when combined with a frequency modulation technique, is a high-resolution Doppler-free tool for probing atoms interacting with a surface. We analyze different types of relevant surface interaction, emphasizing the spectral consequences of a van der Waals surface attraction associated to a z−3z^{-3}z−3 potential dependence (zzz: distance to the wall). We present detailed results of two series of experiments at a Cs vapor/dielectric window interface on the 6S1/2_{1/2}1/2​-6P3/2_{3/2}3/2​ (λ=852\lambda = 852λ=852 nm) resonance line and on the 6S1/2_{1/2}1/2​-7P second resonance line (λ=455\lambda = 455λ=455 nm and 459 nm). Lineshape analysis at various pressures consistently shows that a van der Waals-type surface attraction has to be considered to interpret strong lineshape distortions and resonance shift. The attractive strengths are found to be equal respectively to ≈2\approx 2≈2 kHz μ\muμm3^33 and ≈20\approx 20≈20 kHz μ\muμm3^33, independently of the considered hyperfine component, within the experimental accuracy. It yields also typical parameters of pressure broadening and shift, which are shown to originate in collisional processes, at densities where the medium is opaque. Theoretical expectations for the VW strength are discussed on the basis of the results of atomic theory. The predicted values are smaller, by a typical factor of 2, than those deduced from the experiments. The validity of the theory, when applied to a dielectric interface, is discussed and seems questionable when the frequency of virtual atomic transitions involved in the van der Waals attraction potential lies in the dielectric window absorption range.