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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

Sub-Doppler extra-lines in the vicinity of the 388 nm line of Cs: A signature for dimer photoassociation in a thermal vapour ?

Thierry Passerat de Silans, Isabelle Maurin, Athanasios Laliotis, Daniel Bloch

Published Jun 1, 2009• 1 citation
Publisher

Abstract

The paper reports on the observation of extra sub-Doppler resonance in the vicinity of the third resonance line of Cs (6Srarr8P) at 388 nm (6S1/2rarr8P3/2) and 389 nm (6S1/2rarr8P1/2), when saturated absorption spectroscopy is usually expected to provide a frequency reference in the analysis of other physical processes. All the extra-lines that were detected were located inside the Doppler width, with supplementary components appearing when increasing the irradiating intensities. These observations help to rule out the possibility to explain these observations by a resonant nonlinear optical process, as may occur in the presence of nonlinear processes involving two resonant beams, and mixing- up resonant absorption (or gain) with dispersion. A noticeable difference with photo-association performed with cold atoms is that here, in spite of a velocity-selection induced by saturated absorption, this process is only operated along a single velocity-axis, so that the interaction time between the two atoms that associate is expected to remain extremely short.

DOI
10.1109/cleoe-eqec.2009.5194132

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The absorption and fluorescence spectra of a submicron Cs vapour layer under resonant excitation on the D2 line are measured. Sub-Doppler features centered at the resonance frequency of the hyperfine (hf) transitions have been observed. Substantial changes in the amplitude and width of the sub-Doppler resonances for individual hf transitions were recorded in dependence on the intensity of the incident laser radiation. In the fluorescence spectra narrow dips due to the effects of saturation have been observed. We also report about the observation of coherence resonances in Hanle configuration obtained at cell thickness of the order of the wavelength of the laser light.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Apr 22, 2005•6 citations
The paper reports on the observation of extra sub-Doppler resonance in the vicinity of the third resonance line of Cs (6Srarr8P) at 388 nm (6S1/2rarr8P3/2) and 389 nm (6S1/2rarr8P1/2), when saturated absorption spectroscopy is usually expected to provide a frequency reference in the analysis of other physical processes. All the extra-lines that were detected were located inside the Doppler width, with supplementary components appearing when increasing the irradiating intensities. These observations help to rule out the possibility to explain these observations by a resonant nonlinear optical process, as may occur in the presence of nonlinear processes involving two resonant beams, and mixing- up resonant absorption (or gain) with dispersion. A noticeable difference with photo-association performed with cold atoms is that here, in spite of a velocity-selection induced by saturated absorption, this process is only operated along a single velocity-axis, so that the interaction time between the two atoms that associate is expected to remain extremely short.
We report on the observation of additional sub-Doppler lines in a saturated absorption experiment when exploring the vicinity of the $6{S}_{1/2}\ensuremath{-}8{P}_{3/2}$ transition of Cs (\ensuremath{\lambda}$=$388 nm). These additional lines are observed only under a relatively strong irradiation of both the pump and the probe beams. Extra narrow lines are also observed in copropagating nonlinear spectroscopy, and around the lines of the V-type three-level system $8{P}_{3/2}\ensuremath{-}6{S}_{1/2}\ensuremath{-}8{P}_{1/2}$ (${\ensuremath{\lambda}}_{1}$$=$388 nm, ${\ensuremath{\lambda}}_{2}$$=$389 nm). We attribute theses additional lines to a probing of high-lying molecular cesium, produced as a result of the optical excitation of Cs atoms, as the low Cs atom density (\ensuremath{\le}10${}^{12}cmcmcm{}^{\ensuremath{-}3}$) is unable to populate significantly the dimer states in the condition of thermal equilibrium.
Sub-Doppler resonances in caesium vapours are studied in a laser field produced by counterpropagating two-frequency light beams with mutually orthogonal linear polarisations. The beams are in resonance with optical transitions in the D1 line, the frequency difference of the field spectral components being equal to the hyperfine ground-state splitting in the Cs atom (≈9.2 GHz). It has already been shown that in this configuration, the hypercontrast effect can be observed for sub-Doppler resonances, which makes this configuration promising for the employment in newgeneration miniature optical frequency standards. In the present work, two different two-frequency configurations are compared with each other and with the single-frequency configuration widely used in practice for observing saturated absorption resonances. The parameters of nonlinear resonances are measured at various temperatures of caesium vapours and at different optical field intensities. The results of the investigations performed make it possible to find an optimal two-frequency scheme for exciting nonlinear resonances and to estimate a potential of the scheme for its applications in quantum metrology.
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 .
Abstract Sub-Doppler resonances in caesium vapours are studied in a laser field produced by counterpropagating two-frequency light beams with mutually orthogonal linear polarisations. The beams are in resonance with optical transitions in the D1 line, the frequency difference of the field spectral components being equal to the hyperfine ground-state splitting in the Cs atom (∼9.2 GHz). It has already been shown that in this configuration, the hypercontrast effect can be observed for sub-Doppler resonances, which makes this configuration promising for the employment in new-generation miniature optical frequency standards. In the present work, two different two-frequency configurations are compared with each other and with the single-frequency configuration widely used in practice for observing saturated absorption resonances. The parameters of nonlinear resonances are measured at various temperatures of caesium vapours and at different optical field intensities. The results of the investigations performed make it possible to find an optimal two-frequency scheme for exciting nonlinear resonances and to estimate a potential of the scheme for its applications in quantum metrology.
A new nano-cell with smoothly varying longitudinal thickness of the atomic vapour layer L in the range of 350 - 5100 nm allowing to study the resonant absorption of D1 and D2 lines of Cs atoms for thicknesses changing from L = Lambda/2 to L = 6 Lambda with the step of Lambda/2 (Lambda = 852 nm or 894 nm are the resonant laser wavelengths) and for different intensities is developed. It is revealed that for low laser intensities there is narrowing of the resonant absorption spectrum for the thicknesses L = (2n + 1)Lambda/2 (where n is an integer) up to L = 7Lambda /2 and broadening of the spectrum for L = n Lambda. For relatively high laser intensity (>1 mW/cm2), velocity selective optical pumping/saturated resonances of a reduced absorption (with the line-width close to the natural one), and centred on the hyperfine transitions occur when L = n Lambda. The possible application of these resonance peaks is given. The developed theoretical model describes well the experiment.
The absorption and fluorescence spectra of a submicron Cs vapour layer under resonant excitation on the D2 line are measured. Sub-Doppler features centered at the resonance frequency of the hyperfine (hf) transitions have been observed. Substantial changes in the amplitude and width of the sub-Doppler resonances for individual hf transitions were recorded in dependence on the intensity of the incident laser radiation. In the fluorescence spectra narrow dips due to the effects of saturation have been observed. We also report about the observation of coherence resonances in Hanle configuration obtained at cell thickness of the order of the wavelength of the laser light.