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Journal of Physics Conference Series

Excited atoms-wall collisions and their manifestations in the fluorescence excitation line shapes

T A Vartanayn, S. Cartaleva

Published Jul 1, 2019• 0 citations
Publisher

Abstract

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.

DOI
10.1088/1742-6596/1289/1/012013

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Mar 15, 2013•0 citations
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.
We compare the behavior of absorption and of resonance fluorescence spectra in an extremely thin Rb vapor cell as a function of the ratio of $L∕\ensuremath{\lambda}$, with LLL the cell thickness $(L\ensuremath{\sim}150--1800\phantom{\rule{0.3em}{0ex}}\mathrm{nm})$ and $\ensuremath{\lambda}$ the wavelength of the Rb D2{D}_{2}D2​ line $(\ensuremath{\lambda}=780\phantom{\rule{0.3em}{0ex}}\mathrm{mn})$. The Dicke-type coherent narrowing [G. Dutier et al., Europhys. Lett. 63, 35 (2003)] is observed only in transmission measurements, in the linear regime, with its typical collapse and revival, which reaches a maximum for $L=(2n+1)\ensuremath{\lambda}∕2$ (nnn integer). It is shown not to appear in fluorescence, whose behavior-amplitude, and spectral width, is more monotonic with LLL. Conversely, at high-intensity, the sub-Doppler saturation effects are shown to be the most visible in transmission around $L=n\ensuremath{\lambda}$.
The high resolution spectroscopy of nanometric-thin alkali-vapor layers was made possible through the development of extremely thin cell.We have investigated the behavior of the extremely thin cell fluorescence spectra both experimentally and theoretically.Experiment is performed on the D 2 line of Cs-vapor-layer with thickness L = mλ, where m = 0.5, 0.75, 1, 1.25.For open optical transitions, the fluorescence spectra shows narrow dip on the top of the sub-Doppler-width fluorescence profile, at L ≥ λ.In case of closed transition, an extremely small feature in the fluorescence slightly shifted from its maximum is observed at L = (5/4)λ.The used theoretical model, based on the optical Bloch equations is in qualitative agreement with the experimental observations.
Recently it was demonstrated that miniaturization of alkali cells, i.e. the use of an extremely thin cell (ETC) for the applications using the electromagnetically induced transparency (EIT) effect, despite to intuitive expectation, does not cause a strong broadening of the dark-line (DL) linewidth. Here we present the conditions when a strong broadening of DL linewidth (more than by 10 times) can be easily observed due to atom-wall collisions influence and this could be a convenient and robust tool for atomwall (i.e. ETC's window material/temperature) collisions study. We present experimental and theoretical results on EIT realized in a Λ- system of 85Rb, D2 line, 5S-5P-5S for a Rb vapour column with the thickness L ~ λ (λ = 780 nm) and varying in the range of (0.5 to 6) λ. Two cw diode-lasers (forming the coupling and probe beams) with the linewidths of 1 MHz are used. One of the striking results observed in ETC when the coupling is resonant with the atomic transition is that DL linewidth is weakly dependent on L and this allows us to detect DL at the smallest thickness reported up to now L = 0.5 λ = 390 nm. The explanation is that the contribution of atoms flying parallel to ETC windows is enhanced thanks to their longer interaction time with the laser field. Meanwhile, direct influence of atomwall collisions on DL linewidth is well seen when there is a large detuning Δ of the coupling from the resonant transition. DL linewidth achieves ~100 MHz for the case of Δ ~100 MHz and L ~ λ, meanwhile for the coupling to be resonant, it is < 9 MHz. We present EIT (DL) spectra for different L for the coupling detuned by Δ = 60 MHz from transition Fg =2 →3′ and the probe scanned across Fg=3 → 2′,3′,4′ transitions. In this case only atoms flying in the same direction with the laser radiation participate in the formation of DL and frequent collisions with the walls cause a strong DL broadening.
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.