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Advanced materials research

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

Yuan Li, Li Li, Yi Xin Lu, Xiang Wu Zhang

Published Mar 1, 2013• 0 citations
Publisher

Abstract

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.

DOI
10.4028/www.scientific.net/amr.669.226

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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.
One-photon Dick-narrowing absorption spectroscopy from a thin atomic vapor film can be extended to the two-photon case, in which the sub-Doppler absorption structures are obtained in a cascade three-level system. The periodic line shapes of two photon spectroscopy are similar to one-photon case. It is found that Dicke-narrowing is apparent when L/λ=(2n+1)/2 (n an integer, L the film thickness, and λ the wavelength of the probe field)in the case of one-photon process, and this feature is maintained in the case of two-photon process but not in the one-photon process when L/λ=2n/2. Due to the contribution of atom-wall collision in the cell and the pump-probe scheme, a very narrow structure can be obtained when the pump and the probe fields are in counter-propagation regime.
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#
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.
Understanding the processes underlying the optical excitation of atomic vapor in the vicinity of solid surfaces is of interest both from physical and technical points of view. Selective reflection spectra of laser light from an interface of a transparent dielectric material and resonant vapor are known to be Doppler-free and to provide important spectroscopic information about the atom-wall interaction. On the other hand, atomic vapors have such a large and fast nonlinear response on or near resonances that they are capable of processing signals and images with milliwatt lasers at a time scale of submicroseconds. In the present paper we investigate linear and nonlinear optical properties of a thin film of atomic vapor confined between two solid surfaces. Assuming two-level atoms, we solve the Maxwell- Bloch equations for light reflection from resonant atoms. The interaction between the resonant atoms and the wall is accounted for through the boundary conditions for all elements of density matrix. The transient polarization is shown to make an important contribution not only to the field structure in the vicinity of the wall but also to the interference pattern of the reflected field. It is found that the spectrum of reflection depends remarkably on the film thickness. Strong enhancement of signal is also found from this study and possible devices for the detection 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.
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.