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Optics and Spectroscopy

Comments on the problem of anomalous fluorescence of atomic sodium vapor at a wavelength of 589.6 nm

Н. И. Косарев

Published Jul 1, 2006• 5 citations
Publisher

Abstract

The problem of the laser-induced fluorescence of sodium vapor at a wavelength of 589.6 nm in the case of photoexcitation of a small volume of the medium by a laser beam has been solved numerically. The photon transfer from the zone of excitation to the periphery in the direction perpendicular to the direction of propagation of the laser radiation leads to a significant extension of the volume with a high density of excited atoms. The influence of this factor on the formation of the resonance fluorescence of sodium vapor is discussed.

DOI
10.1134/s0030400x06070113

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The problem of the laser-induced fluorescence of sodium vapor at a wavelength of 589.6 nm in the case of photoexcitation of a small volume of the medium by a laser beam has been solved numerically. The photon transfer from the zone of excitation to the periphery in the direction perpendicular to the direction of propagation of the laser radiation leads to a significant extension of the volume with a high density of excited atoms. The influence of this factor on the formation of the resonance fluorescence of sodium vapor is discussed.
Abstract The problem of transfer of line radiation in sodium vapor under photoexcitation by laser radiation of a resonance line with wavelength λ = 589.6 nm is numerically solved. The influence of Doppler frequency shifts on photon emission coherent in the atomic reference system is taken into account in the formation of an emission line profile using the model of partial frequency redistribution. In the case of a small optical thickness of a medium τ0 ≤ 1, the Doppler frequency redistribution in the laboratory reference system yields higher intensity values in the emission line profile core in comparison with the model of complete frequency redistribution. For an optically dense medium, thermal motion of atoms leads to an increase of reabsorption in the emission line core, and intensity increases in the line wings as compared to the complete redistribution model. The dependence of the Holstein trapping factor on optical thickness is closer to the analytic dependence than the complete redistribution model. This is explained by the fact that the frequencies of emitted photons in the laboratory reference system fall into the spectral profile core, which increases the effects of resonance radiation trapping in a dense medium.
We describe the influence of radiation trapping on the spatial distribution of the excited-state population in sodium vapor, interacting with a linearly polarized Gaussian laser beam. Counterintuitively the excitation volume experiences a strong spatial shrinking at high optical depth. The interpretation of this nonlocal effect is based on the numerical solution of the stationary Holstein equation, which takes into account the full frequency dependence of the reabsorption probability within the process of diffusion of radiation. The calculations performed are in good qualitative agreement with the spatial effects observed experimentally. \textcopyright{} 1996 The American Physical Society.
Laser-induced fluorescence (LIF) was studied in the 400–1000 nm wavelength range using narrow-band 852 nm laser radiation resonant with Cs atomic 6S1/2 → 6P3/2 transition. T-shaped cells made entirely of technical sapphire with thicknesses of L = 1 cm, 40 μm, and ~400 nm, containing cesium atomic vapor, were used. It was shown that with the cell thickness decrease (from centimeters to nanometer thicknesses), many LIF signals are suppressed due to an increase in the number of atomic collisions with the walls, leading to quenching of excited states. By recording the LIF signal, it is also possible to estimate the amount of residual Rb atomic vapor (if any exists) in the Cs-containing cell. The Cs vapor cell can serve as an efficient optical frequency converter filter and has other applications.
An experimental and theoretical investigation is made of the angular spectrum of a near-resonant femtosecond laser pulse propagating through sodium vapor. A directional fluorescence emission corresponding to single-photon sodium transition $3S\ensuremath{\rightarrow}3{P}_{1∕2,3∕2}$ has been registered for the pump wavelength ranging from 540to605nm540\phantom{\rule{0.3em}{0ex}}\text{to}\phantom{\rule{0.3em}{0ex}}605\phantom{\rule{0.3em}{0ex}}\mathrm{nm}540to605nm. It is found that such emission can be detected under the conditions of single-photon (enhanced by two-photon) resonance of pump frequency with relevant atomic states. Theoretical treatment of the field-matter interaction by means of the nonperturbative (semiclassical) approach revealed conical components of the cylindrically symmetric beam spectrum originating both from the fluorescence induced by coherent atomic polarization and four-wave mixing.
The thermal luminescence spectra of a dense, nonuniformly heated resonance medium (sodium vapor) are investigated experimentally under conditions when the resonance corrections to the relative permittivity are not small compared to unity and the photon mean free path is comparable to the wavelength of the radiation. The shape of the recorded spectra agrees well with a previously developed general theory of resonance radiation transfer which predicts a strong asymmetry of the spectra. The prospects for performing more-sensitive measurements in order to make a quantitative check of the theoretically predicted anomalous intensity (an order of magnitude higher than in the standard theory of resonance radiation transfer) of the radiation from a dense nonuniform medium are discussed.
Measurements are reported which show the effect of nonradiative losses at a gas-window interface on the backscattered fluorescence intensity for Na vapor at frequencies in the vicinity of the resonance lines near 589 nm. The Na 3P12,323{P}_{\frac{1}{2},\frac{3}{2}}3P21​,23​​ states are excited with a low-intensity single-mode tunable dye laser at high Na densities and the frequency integral of the backscattered fluorescence intensity in the D1D1D1 and D2D2D2 lines is measured. As the laser is tuned through resonance, the loss of atomic excitation to the window appears as a sharp decrease in the frequency-integrated fluorescence intensity. For example, at 7\ifmmode\times\else\texttimes\fi{}1020{10}^{20}1020 atoms ${\mathrm{m}}^{\ensuremath{-}3}$ the fluorescence intensity decreases by a factor of 4 in a frequency interval of 4 GHz. Measured absolute fluorescence intensities versus laser frequency are compared with predictions made using the theory of Hummer and Kunasz which includes both radiative and nonradiative transport processes. The agreement between theory and experiment is remarkably good when one considers that the theory contains only one unknown coefficient, i.e., the reflection coefficient for excited atoms at the windows. In our case the excited atoms are assumed to be completely destroyed at the window.