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Contemporary Physics

The fluorescence of atoms near a glass surface

Martin F. H. Schuurmans

Published Sep 1, 1980• 17 citations
Publisher

Abstract

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.

DOI
10.1080/00107518008210971

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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.
When a vapour is confined, the collisions to the confinement wall usually cause a broadening of the transitions. However velocity selective processes and the coherent enhancement of some transient contributions can lead to sub-Doppler contributions because of the confinement. In the optical range, this had been demonstrated for a one-dimensional confinement with micro- or nano-cells of a small thickness. A two-dimensional confinement in a hollow fiber had shown sub-Doppler contributions, but only equivalent to macrosocpic non linear saturated absorption spectroscopy. Here, we describe experiments showing that a thermal vapor confined in a three-dimensional nanostructure can exhibit sub-Doppler features in a linear regime. We perform reflection spectroscopy on a Cs vapour cell whose window is covered with a thin opal film (typically, 10 or 20 layers of ~ 1µm or 400 nm diameter spheres). We demonstrate, both experimentally and through a modeling that the sub-Doppler structures observed for a large range of oblique incidence angles (~ 30-50°) originate from the interstitial regions of the opal, hence corresponding to a three-dimensional submicrometric confinement. We also show that the partially porous nature of the glass spheres allows some LIAD effects. In a different set of experiments, an atomic vapour is confined in glass medium with large size pores (tens of µm) randomly distributed. The effect of scattered light and fluorescence have been distinguished. Also, sub-Doppler features evolving non linearly with the irradiating intensity are observed, originating in a saturated absorption process induced by the backscattered light .
Ultra-narrow cells with the thicknesses in the range from several wavelengths to the small fractions of the wavelength brought a number of new opportunities for atomic spectroscopy. Depending on the cell thickness, spectral lines recorded in ultra-narrow cells are either Doppler-free or Doppler-broadened. With careful selection of the cell thickness hyperfine structure may be easily resolved without resorting on the multibeam nonlinear optical techniques. Moreover, frequent collisions with the walls leads to the important modifications of velocity selective optical pumping resonances. Finally, ultra-narrow cells provide with the unique opportunity to study collisions of the excited atoms with the solid surfaces. In this contribution several examples of the use of the ultra-narrow spectroscopic cells filled with the alkali atomic vapour is presented. First, we discuss general aspects of the transient polarisation that defines all peculiarities of an ultra-narrow cell as a spectroscopic tool. Second, we demonstrate the resolution of the magnetic sublevels in the transition from Zeeman to Paschen-Back regime in the Cs hyperfine structure. Third, new aspects of velocity selective optical pumping resonances in reflection and transmission of resonant radiation by the 6 wavelengths thick cell filled with Cs are discussed. Forth, the experimental evidences of the nonadiabatic transitions between excited states of Rb atoms in the course of collisions with the sapphire surface are presented.
Since the invention of the extremely thin cell which sustains prolonged action of hot and dense alkali vapours, a number of spectroscopic problems have been solved with its aid. As the width of the cell is comparable to, or smaller than, the wavelength of the actual atomic transition, The Doppler width of the fluorescence light is reduced due to the cage effect. Stimulated by recent measurements of the fluorescent excitation line shapes in the extremely thin cell we studied the dependence of these line shapes on the cell thickness.
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.