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AIP conference proceedings

Linear and nonlinear selective reflection spectroscopy

Anne Amy‐Klein, O. A. Rabi, Solomon M. Saltiel, Nicolas Papageorgiou, M. Fichet, Daniel Bloch, Vladimir A. Sautenkov, Antoine Weis, M. Ducloy

Published Jan 1, 1993• 0 citations
Publisher

Abstract

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.

DOI
10.1063/1.45029

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Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics•Mar 27, 2001•21 citations
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.
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.
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 calculate the modulation of the reflection coefficient for a frequency-modulated (FM) light beam incident on the interface between a dielectric and an atomic vapor. The vapor is described as a gas of resonant, Doppler-broadened, two-level systems, with transition frequency and linewidth arbitrarily depending on the atom-dielectric distance. The atoms are supposed to get deexcited at collisions with the surface. The transient atomic response is calculated to first order in the incident field, for both incoming and desorbed atoms. The reflection coefficient, evaluated to first order in the vapor dipole polarization, leads to a formal expression of the reflectivity modulation, valid for arbitrary atom-surface interaction potentials. One first discusses the reflection signal in absence of wall interactions, for arbitrary modulation frequencies. At large frequencies, it allows one to monitor both vapor absorption and dispersion. Second, the formal theory is applied to the case of a Van der Waals-London surface attraction exerted on the atomic vapor. Both normal and oblique beam incidences are considered. One shows how the vapor dispersion signal is red-shifted and strongly distorted by the appearance of vapor-surface long-range interactions, and how it can be used to monitor these interactions. At non-normal incidences, the lineshapes get Doppler-broadened.
Frequency-modulated selective-reflection spectroscopy of the 6S-7P Cs resonance line yields Doppler-free anomalous line shapes that we demonstrate to be fully dominated by the long-range atom-surface interaction potential. The spatial inhomogeneous broadening of the observed line shapes, as well as its dependence on the pressure, the nature of the dielectric window, and the light incidence angle, is fully interpreted with a z(-3) van der Waals attraction model. These experiments clearly prove the feasibility of a spectral analysis of atom-surface interactions.
The atomic response to resonant light irradiation near vapor-dielectric interfaces is monitored via high-resolution reflection spectroscopy. One demonstrates that this Doppler-free spectroscopic technique yields a novel probe of atomic dynamics and QED atom-surface long- range interaction. It provides for the first time a spectral evidence of van der Waals attraction, and the method is intrinsically applicable to the observation of surface interaction exerted on excited atoms. Effects related with atomic excitation level, nature of the dielectrics, and atomic collisions are discussed.
We discuss the properties of selective reflection spectroscopy at the interface between a resonant vapor and a complex dense medium, such as a metallic film layered on a dielectric substrate. We show that in the approximation of a low-density vapor, the signal mixes up the absorptive and dispersive components of the "effective resonant susceptibility" of the vapor, with the mixture amount governed by simple laws of linear optics. Preliminary experiments performed at the interface between Cs vapor (D2, 852-nm line) and a silver-coated glass window are reported, that show qualitatively the effect of the atom-surface van der Waals interaction.