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. \textcopyright{} 1996 The American Physical Society.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. \textcopyright{} 1996 The American Physical Society.

Physical Review AOct 1, 199614 citations

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

Anne Amy‐Klein, Solomon M. Saltiel, O. A. Rabi +1 more

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.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.

Physical Review AOct 1, 199513 citations

Selective reflection from a vapor of three-level atoms

Gerard Nienhuis, F. Schuller

We study internal selective reflection from a dielectric-vapor interface, where three levels of the vapor atoms in a \ensuremath{\Lambda} configuration are connected by two light frequencies. The reflectivity contains then both a sub-Doppler structure due to spatial dispersion in the boundary layer and the dark resonance arising from coherent population trapping. We derive analytical expressions for the reflectivity of either one of the two light beams. The contributions from atoms approaching or leaving the interface are strongly different, whereas they are identical for the case of two-state atoms.We study internal selective reflection from a dielectric-vapor interface, where three levels of the vapor atoms in a \ensuremath{\Lambda} configuration are connected by two light frequencies. The reflectivity contains then both a sub-Doppler structure due to spatial dispersion in the boundary layer and the dark resonance arising from coherent population trapping. We derive analytical expressions for the reflectivity of either one of the two light beams. The contributions from atoms approaching or leaving the interface are strongly different, whereas they are identical for the case of two-state atoms.

Physical Review AAug 1, 199417 citations

Saturation effects in three-level selective reflection

F. Schuller, Anne Amy‐Klein, Solomon M. Saltiel

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 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.

Physical Review AMay 1, 19965 citations

Two-Photon Selective Reflection Spectroscopy of Confined Atomic Vapor at the Interface with a Ferroelectric Layer

Yuan Li, Li Li, Yi Xin Lu +1 more

We examine two-photon selective reflection (SR) spectroscopy in a system of -type three-level atoms at the interface with a ferroelectric layer on a dielectric surface. Two-photon SR lines, exhibiting Dicke-narrowing profiles due to atom-wall collision and Doppler free configuration, are periodically modulated by the thickness of the atomic vapor. These SR lines can be modified by the thickness and the complex refractive index of the ferroelectric layer, and can probably be a feasible method used in the measurement of the optical parameters of the ferroelectric layer.We examine two-photon selective reflection (SR) spectroscopy in a system of -type three-level atoms at the interface with a ferroelectric layer on a dielectric surface. Two-photon SR lines, exhibiting Dicke-narrowing profiles due to atom-wall collision and Doppler free configuration, are periodically modulated by the thickness of the atomic vapor. These SR lines can be modified by the thickness and the complex refractive index of the ferroelectric layer, and can probably be a feasible method used in the measurement of the optical parameters of the ferroelectric layer.

Advanced materials researchMar 1, 20130 citations

Nonlinear selective reflection in cascade three-level atomic systems

F. Schuller, O. Gorceix, M. Ducloy

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 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.

Physical Review AJan 1, 199338 citations

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}

{\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.