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Optics Letters

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, M. Ducloy

Published Dec 1, 1991• 42 citations
Publisher

Abstract

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.

DOI
10.1364/ol.16.001879

Related papers

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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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.

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General theory of frequency modulated selective reflection. Influence of atom surface interactions

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We report on the analysis of FM selective reflection experiments on the 6S1/2->8P3/2 transition of Cs at 388 nm, and on the measurement of the surface van der Waals interaction exerted by a sapphire interface on Cs(8P3/2). Various improvements in the systematic fitting of the experiments have permitted 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. We finally 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 vW interaction for Cs(8P3/2) lie in the far infrared range.

•Jan 26, 2007•0 citations

Quantum optics at vapor-dielectric interfaces

Martine Chevrollier, M. Fichet, Marcos Oriá +2 more

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.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Oct 28, 1992•0 citations
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.
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 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.
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.
We report on the analysis of FM selective reflection experiments on the 6S1/2->8P3/2 transition of Cs at 388 nm, and on the measurement of the surface van der Waals interaction exerted by a sapphire interface on Cs(8P3/2). Various improvements in the systematic fitting of the experiments have permitted 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. We finally 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 vW interaction for Cs(8P3/2) lie in the far infrared range.
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.