Sub-Doppler spectroscopy of gaseous media confined in thin pillbox-shaped cells was pioneered by R.H. Dicke. In the past, this idea attracted much less attention compared to "Dicke narrowing" in buffer gas where the atoms or molecules perform a diffusive motion instead of being bounced back and forth between the walls of the cell in a completely predetermined nature. The situation is going to be changed as atomic spectroscopy becoming an essential part of mobile devices for civil and military applications that require tiny spectroscopic cells. In the pillbox shaped cells, the role of the fast moving atoms is diminished, while the slowly moving atoms contribute most to the absorption as well as to the fluorescence. The role of the slowly moving atoms and their transient polarization in selective reflection spectroscopy was highlighted by J.L. Cojan. By merging these two approaches we have developed a theoretical description of optical reflection from and transmission through the narrow slice of atomic vapours.
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.
Selective reflection spectroscopy at an interface with a low-density resonant vapor, especially when combined with a frequency modulation technique, is a high-resolution Doppler-free tool for probing atoms interacting with a surface. We analyze different types of relevant surface interaction, emphasizing the spectral consequences of a van der Waals surface attraction associated to a
z−3 potential dependence (
z: distance to the wall). We present detailed results of two series of experiments at a Cs vapor/dielectric window interface on the 6S
1/2-6P
3/2 (
λ=852 nm) resonance line and on the 6S
1/2-7P second resonance line (
λ=455 nm and 459 nm). Lineshape analysis at various pressures consistently shows that a van der Waals-type surface attraction has to be considered to interpret strong lineshape distortions and resonance shift. The attractive strengths are found to be equal respectively to
≈2 kHz
μm
3 and
≈20 kHz
μm
3, independently of the considered hyperfine component, within the experimental accuracy. It yields also typical parameters of pressure broadening and shift, which are shown to originate in collisional processes, at densities where the medium is opaque. Theoretical expectations for the VW strength are discussed on the basis of the results of atomic theory. The predicted values are smaller, by a typical factor of 2, than those deduced from the experiments. The validity of the theory, when applied to a dielectric interface, is discussed and seems questionable when the frequency of virtual atomic transitions involved in the van der Waals attraction potential lies in the dielectric window absorption range.
Frequency-modulated selective-reflection spectroscopy of the 6S-7P Cs resonance line yields Doppler-free anomalous line shapes that we demonstrate to be fully dominated by the long-range atom-surface interaction potential. The spatial inhomogeneous broadening of the observed line shapes, as well as its dependence on the pressure, the nature of the dielectric window, and the light incidence angle, is fully interpreted with a z(-3) van der Waals attraction model. These experiments clearly prove the feasibility of a spectral analysis of atom-surface interactions.
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.
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.