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Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics

Selective reflection spectroscopy of a resonant vapor at the interface with a metallic layer

Martine Chevrollier, Marcos Oriá, Janete Gouveia de Souza, Daniel Bloch, M. Fichet, M. Ducloy

Published Mar 27, 2001• 21 citations
Publisher

Abstract

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.

DOI
10.1103/physreve.63.046610

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High resolution selective reflection spectroscopy as a probe of long-range surface interaction : measurement of the surface van der Waals attraction exerted on excited Cs atoms

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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 $z^{-3}$ potential dependence ($z$: distance to the wall). We present detailed results of two series of experiments at a Cs vapor/dielectric window interface on the 6S$_{1/2}$-6P$_{3/2}$ ($\lambda = 852$ nm) resonance line and on the 6S$_{1/2}$-7P second resonance line ($\lambda = 455$ 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 $\approx 2$ kHz $\mu$m$^3$ and $\approx 20$ kHz $\mu$m$^3$, 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.

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Van der Waals-induced spectral distortions in selective-reflection spectroscopy of Cs vapor: the strong atom–surface interaction regime

Martine Chevrollier, Daniel Bloch, G. Rahmat +1 more

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.

Optics Letters•Dec 1, 1991•42 citations
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.
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 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.
We report on the analysis of FM selective reflection experiments on the 6S 1/2 → 8P 3/2 transition of Cs at 388 nm, and on the measurement of the surface van der Waals interaction exerted by a sapphire interface on Cs(8P 3/2). Various improvements in the systematic fitting of the experiments have permitted us to supersede the major difficulty of a severe overlap of the hyperfine components, originating, on the one hand, in a relatively small natural structure, and, on the other hand, on a large pressure broadening imposed by the high atomic density needed for the observation of selective reflection on a weak transition. The strength of the van der Waals surface interaction is evaluated to be 73 ± 10 kHz µm3. An evaluation of the pressure shift of the transition is also provided as a by-product of the measurement. Finally, we discuss the significance of an apparent disagreement between the experimental measurement of the surface interaction, and the theoretical value calculated for an electromagnetic vacuum at a null temperature. The possible influence of the thermal excitation of the surface is evoked, because the dominant contributions to the van der Waals interaction for Cs(8P 3/2) lie in the far-infrared range.
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.