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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Multiphoton evanescent wave spectroscopy and dynamics

Vladimir G Bordo, Horst‐Guenter Rubahn

Published Dec 5, 2001• 0 citations
Publisher

Abstract

Non-intrusive laser-spectroscopical methods for the diagnostics of the gas-surface interaction in the near-field of a dielectric surface have been developed both experimentally and theoretically. The techniques base on either two-photon evanescent wave excitation or combined evanescent-volume wave excitation. Spectra obtained for sodium atoms at a glass-vacuum interface are quantitatively reproduced by a rigorous theoretical approach. In the case of pure evanescent wave excitation the excitation conditions can be chosen such that either the velocity distribution of desorbing atoms is determined or that atom-surface interaction parameters (polarizability of the adsorbed atoms, desorption rate, sticking coefficient) are obtained from the Autler- Townes splitting of the two-photon lines. By the use of combined evanescent-volume wave excitation one is able to distinguish optically between different groups of atoms interacting with the surface and one can extract their two- dimensional velocity distributions. In addition, information is obtained about superelastic scattering of the atoms interacting with the dielectric substrate.

DOI
10.1117/12.449526

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Non-intrusive laser-spectroscopical methods for the diagnostics of the gas-surface interaction in the near-field of a dielectric surface have been developed both experimentally and theoretically. The techniques base on either two-photon evanescent wave excitation or combined evanescent-volume wave excitation. Spectra obtained for sodium atoms at a glass-vacuum interface are quantitatively reproduced by a rigorous theoretical approach. In the case of pure evanescent wave excitation the excitation conditions can be chosen such that either the velocity distribution of desorbing atoms is determined or that atom-surface interaction parameters (polarizability of the adsorbed atoms, desorption rate, sticking coefficient) are obtained from the Autler- Townes splitting of the two-photon lines. By the use of combined evanescent-volume wave excitation one is able to distinguish optically between different groups of atoms interacting with the surface and one can extract their two- dimensional velocity distributions. In addition, information is obtained about superelastic scattering of the atoms interacting with the dielectric substrate.
A new spectroscopic technique for studying adsorption of atoms at a transparent dielectric surface is exploited. A quantitative comparison of the Autler-Townes splitting in measured and calculated, surface temperature-dependent two-photon evanescent wave spectra provides values of the adsorption energy, the preexponential factor for the rate of desorption and the polarizability of alkali atoms, adsorbed on a glass surface. It is speculated that this technique could form the basis for future two-photon control of atoms close to dielectric surfaces.
We present a new spectroscopic technique which utilizes evanescent waves at a gas/glass prism interface for studying adsorption/desorption processes. We have measured the Autler-Townes splitting in the two-evanescent wave fluorescence spectrum of Na atoms in the gas phase as a function of the temperature of a prism surface. A quantitative comparison of measured with calculated spectra has provided values of the adsorption energy, pre-exponential factor for the rate of desorption and linear polarizability of adsorbed Na atoms. A possible extension of this technique to the case of surface plasmon excitation at a metal surface is also exploited.
Up to now, Doppler-free nonlinear spectroscopy has been applied to atoms inside a gas medium (volume spectroscopy). We have extended these methods to atoms in the vicinity of a surface. The basic principle consists of monitoring reflectivity changes produced when a laser beam, incident on a glass–vapor interface, is brought into resonance with an atomic transition. For Doppler-free spectroscopy, two counterpropagating beams are used to operate velocity selection. If these two beams are under normal incidence in the glass—velocity selection perpendicular to the surface—one observes saturated dispersion (selective reflection sensitive to the real index). For incidence angles in the glass (prism) larger than the critical angle (total internal reflection), a standing evanescent wave is produced in the gas (velocity selection along the surface), and saturated absorption is detected. Experimental demonstration was performed on the Na resonance line; high sensitivity (10−4 relative reflectivity change) and spectral resolution as good as 20 MHz were obtained. The main limitation to better resolution comes from the short atomic transit time in the evanescent wave (typical extension ~λ). Relevant applications of these techniques should also concern the diagnostics of optically thick media, as analysis of interaction between gas-phase atoms and the surface, notably atom–wall collisions, and modification of the spontaneous emission characteristics.
The two-photon spectrum of sodium atoms, excited by two counterpropagating evanescent waves, is investigated both experimentally and theoretically. Sub-Doppler linewidths are observed, which are quantitatively reproduced by a rigorous theoretical approach that takes into account optical pumping and transit time broadening due to the translational motion of the arriving and departing atoms through the evanescent-wave fields. The velocity distribution of the atoms desorbing from the surface is found to obey a cosine law, which has a significant influence on the observed line shapes.
The gas-surface scattering kernel for Na atoms interacting with a dielectric surface is obtained by measuring and theoretically reproducing two-photon evanescent-volume-wave spectra. From a detailed analysis of the spectral line shapes the contribution of inelastically scattered atoms is identified and a mean energy transfer of 36 meV is deduced for atoms having initial mean thermal energies of 79 meV. The mean probability of direct scattering mediated by surface phonons increases from 0.03 to 0.05 by increasing the surface temperature from 386 K to 398 K.
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.