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Physical Review A

Transient behavior of optically excited vapor atoms near a solid interface as observed in evanescent wave emission

A.L.J. Burgmans, Martin F. H. Schuurmans, Bouwe Bolger

Published Nov 1, 1977• 25 citations
Publisher

Abstract

Using a cw dye laser beam normally incident on a glass-Na-vapor interface, fluorescence excitation spectra of the ${D}_{1}$ line are measured. By observing the fluorescence transmitted into the glass above the angle of total reflection, only evanescent light emitted within about a wavelength distance from the interface is observed. The measured spectra show a cutoff on the high-frequency side which is direct evidence for the transient behavior of the induced polarization of resonantly excited vapor atoms which have collided at the solid interface.

DOI
10.1103/physreva.16.2002

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Using a cw dye laser beam normally incident on a glass-Na-vapor interface, fluorescence excitation spectra of the D1{D}_{1}D1​ line are measured. By observing the fluorescence transmitted into the glass above the angle of total reflection, only evanescent light emitted within about a wavelength distance from the interface is observed. The measured spectra show a cutoff on the high-frequency side which is direct evidence for the transient behavior of the induced polarization of resonantly excited vapor atoms which have collided at the solid interface.
The penetration depth and pseudomomentum (wave vector) of evanescent electromagnetic waves are measured at a planar dielectric surface by means of laser spectroscopy using the Cs D2{\mathrm{D}}_{2}D2​ line with a wavelength of 852.1 nm. The same experimental setup is employed in all the experiments. The first result shows a sharp, asymmetric absorption profile, which is explained in terms of the thin penetration depth, and the second shows an actual transfer of the pseudomomentum of the surface electromagnetic mode to atoms via a resonance interaction. The measured penetration depth and pseudomomentum agree with the natural interpretation of the complex wave number characterizing evanescent waves at a planar dielectric-vapor interface. Direct excitation of evanescent waves by excited Cs atoms has also been observed as atomic fluorescence emitted into the dielectric material at the angle of total internal reflection. The results are in good agreement with the theoretical predictions and exhibit the characteristics of excitation transfer or tunneling from Cs atoms into the surface mode.
Fluorescence spectra of atomic vapours may contain sub-Doppler structure due to the transient behaviour of the light-induced polarization of atoms which have just collided at the wall of the cell containing the vapour. This structure arises in spectra measured in reflection and in emission produced by atoms within a wavelength distance from the entrance window of the cell. Excitation spectra of transmitted light and laterally scattered light are not affected by the atom–wall collisions. Absorption and dispersion of light in an atomic vapour is conventionally described by a complex-valued and frequency-dependent index of refraction. In the presence of atom–wall collisions this theoretical description fails. This report gives an account of how the theory may be modified to include atom–wall collisions; it is assumed that the induced polarization of an atom is lost in such collisions. The modified theory qualitatively describes the experimental results. We review the conventional theory, the modified theory and the experiments featuring sub-Doppler structure related to the transient polarization behaviour.
We compare the interactions of spin-polarized Na with glass surfaces that are either bare or silicone coated. For this purpose, we reflect a laser beam that is resonant with the Na atoms from the interface, using an angle of incidence close to the critical angle of total internal reflection. Polarization-selective detection of the reflected light provides information about the ground-state orientation of the atoms, which is created by optical pumping with a second laser beam. Our theoretical description treats the atomic vapor as a homogeneous anisotropic medium characterized by a macroscopic magnetization. Comparative experimental studies performed with silicone-coated and bare glass surfaces provide evidence that wall relaxation can be observed by reflection spectroscopy.
We calculate the reflection coefficient for a light beam incident on the interface between a dielectric and a resonant atomic vapor to first order in the dipole polarization in the vapor. The angle of incidence and the polarization direction are chosen arbitrarily, and saturation is fully accounted for. The atoms are supposed to get deexcited at collisions with the surface. The resulting transient behavior of atoms leaving the surface is responsible for a nonlocal response. This spatial dispersion near the surface is known to produce a natural-linewidth-limited resonance in the vapor reflection coefficient at normal incidence. Our analysis shows that this sub-Doppler structure is broadened by the residual Doppler effect for non-normal incidence. This structure disappears at the critical angle for total internal reflection, where one predicts a conventional Voigt-type dispersion response, based on the complex-refractive-index approach. We also calculate the saturation broadening of the atomic response for large intensities. Beyond the critical angle, the spectral response suddenly shifts from dispersion to absorption line shapes. In the case of total internal reflection, the spatial dispersion leads to an additional Lorentzian broadening, which results from an effective imaginary Doppler shift at passage through the evanescent wave (transit-time broadening).
Measurements are reported which show the effect of nonradiative losses at a gas-window interface on the backscattered fluorescence intensity for Na vapor at frequencies in the vicinity of the resonance lines near 589 nm. The Na 3P12,323{P}_{\frac{1}{2},\frac{3}{2}}3P21​,23​​ states are excited with a low-intensity single-mode tunable dye laser at high Na densities and the frequency integral of the backscattered fluorescence intensity in the D1D1D1 and D2D2D2 lines is measured. As the laser is tuned through resonance, the loss of atomic excitation to the window appears as a sharp decrease in the frequency-integrated fluorescence intensity. For example, at 7\ifmmode\times\else\texttimes\fi{}1020{10}^{20}1020 atoms ${\mathrm{m}}^{\ensuremath{-}3}$ the fluorescence intensity decreases by a factor of 4 in a frequency interval of 4 GHz. Measured absolute fluorescence intensities versus laser frequency are compared with predictions made using the theory of Hummer and Kunasz which includes both radiative and nonradiative transport processes. The agreement between theory and experiment is remarkably good when one considers that the theory contains only one unknown coefficient, i.e., the reflection coefficient for excited atoms at the windows. In our case the excited atoms are assumed to be completely destroyed at the window.
Absorption spectrum of the evanescent light at a glass/Rb vapor interface has been observed with atom density from 9 ×10 19 m -3 to 5 ×10 20 m -3 . Absorption is as high as 60% at the peak of a hyperfine structure split line. The absorption spectrum of the experiment is compared with that of the calculation based on Fresnel's relation on the assumption of a homogeneous electric susceptibility of the vapor. Near the critical angle the calculation which incorporates the Lorentz–Lorenz local-field correction reproduces the experimental red shift only partly.