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Journal of Physics Conference Series

Spectroscopy of Atomic Vapors in Nanometer Cells: Dicke Narrowing and Beyond

T. A. Vartanyan, V. V. Khromov

Published Dec 6, 2012• 2 citations
Publisher

Abstract

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.

DOI
10.1088/1742-6596/397/1/012059

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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.
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.
Atom-wall interactions play an unexpectedly important role in the atomic spectroscopy. J.L. Cojan was the first who observed and then interpreted the effects of the atom-wall interactions on the reflection spectra in the vicinity of the atomic spectral line. His observation was made on the mercury vapors of such a low concentration that the Doppler width was much larger than the homogeneous width of the atomic transition. Surprisingly, the width of the spectral line he observed in reflection was much smaller than the Doppler width. He pointed out that the atoms those leave the window posses a transient rather than the stationary polarization. This is the reason why their contribution to the reflected field differs from what was expected. M. Ducloy employed the tiny distortions of these narrow resonances in reflection spectra to measure for the first time the van der Waals constants in the excited atomic states. In our work we considered reflection from a narrow slice of atomic vapors and found a manifold of spectral line shapes depending on the width of the vapor slice that have nothing in common with the Fabri-Perot resonances. It was not until the invention of an Extremely Thin Cell (ETC) by D. Sarkisyan that the observation of these effects becomes possible in the optical domain. In the subsequent years ETC proved to be a very powerful tool of modern spectroscopy.
Transmission sub-Doppler spectroscopy with confined atomic vapor film between two dielectric walls is theoretically studied. Because of atoms flying from wall to wall, where they get de-excited, the atom-field interaction time is anisotropic so that the contribution of slow atoms is enhanced, a sub-Doppler transmission spectroscopy (Dicke narrowing effect) can be obtained when the thickness of the film is much small or comparable with the wavelength even at small angle oblique incidence. It is feasible to get a sub-Doppler structure in a new region (L < ?/4) in experiments.
We show that a thermal vapor confined in a nanostructure is of spectroscopic interest. 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 diameter spheres). Sub-Doppler structures appear in the optical spectrum in a purely linear regime of optical excitation and the signal is shown to originate from the interstitial regions of the opal. These narrow spectral structures, observable for a large range of oblique incidence angles (~ 30-50°), are an original feature associated to the 3-D vapor confinement. It remembers a Dicke narrowing, i.e. a Doppler broadening suppression when the atomic motion is sub-wavelength confined. This narrowing, commonly observed in the r.f. domain when a buffer gas ensures a collision confinement effect, had remained elusive in the optical frequency. Also, we describe preliminary experiments performed in a pump-probe technique, intended to elucidate the spatial origin of the narrow contribution. We finally discuss how our results allow envisioning micron-size references for optical frequency clocks, and high resolution spectroscopy of weak and hard-to-saturate molecular lines.
Spectral lineshape narrowing of atomic vapour emission in a bufferless, wall-coated absorption cell has been analysed using the same formalism developed to describe sub-Doppler linewidths, Dicke narrowing, in a buffered cell. Within this formalism lineshapes are generated using Monte Carlo techniques. Dramatic linewidth reductions in the bufferless cell, compared with the buffered cell, occur because of the high probability that Doppler shifts before and after a particular wall collision will cancel each other. The formalism described allows more physical insight than the classic one-dimensional box model previously invoked to explain spectra narrowing in bufferless, wall-coated cells. Additionally, this formalism reveals a correlation between post-collision velocities and intercollision times in the buffered cell resulting in modifications of the standard Dicke analysis of these cells.
Single light beam transmission spectroscopy in an ultrathin dilute vapor cell (10--100 \ensuremath{\mu}m) reveals sub-Doppler features. Indeed, atoms with fast (normal) velocity undergo a short interaction between the cell walls, and are shown to be less absorbing because they have not reached their steady state of interaction with light. The effect is observed in the linear-response regime with a simple two-level system, as ensured from the ultralow level of light irradiation ($<~1\ensuremath{\mu}{\mathrm{W}/\mathrm{c}\mathrm{m}}^{2}$ for the Cs D2{D}_{2}D2​ line). The effect, known for a long time in the microwave domain, is demonstrated here in the optical domain, and is extended to cell thicknesses large relative to the optical wavelength.