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Physical Review A

Radiation diffusion and saturation in optically thick Na vapor

John Huennekens, Alan C. Gallagher

Published Jul 1, 1983• 69 citations
Publisher

Abstract

We have measured the time-dependent fluorescence of the sodium $D$ lines following pulsed excitation of one $D$ line, in the presence of radiation trapping with optical depths ${k}_{0}L$ of \ensuremath{\sim}10 to 2000. When collisional coupling of the $3{P}_{\frac{1}{2}}$ and $3{P}_{\frac{3}{2}}$ levels and different radiative-escape probabilities for each $D$ line are taken into account, we obtain excellent agreement with Holstein's theory for the effective radiative decay rates in the Doppler region (${k}_{0}L\ensuremath{\sim}10\ensuremath{-}300$) and in the redistributed Lorentzian region (${k}_{0}L>1000$). For ${k}_{0}L$ between these two regions, we observe an abrupt transition between the two limiting formulas. The buildup rate of the sensitized fluorescence signal also yields a $3{P}_{\frac{3}{2}}\ensuremath{\rightarrow}3{P}_{\frac{1}{2}}$ excitation transfer cross section in agreement with our previously reported cw measurement. Additionally, we have measured the dependence of the $3P$ fluorescence on laser power and beam diameter, and we explain the observed approach to saturation. We suggest that the previously reported "anomalous" approaches to saturation may be explained in terms of the laser beam burning through the optically thick vapor. Laser-beam spatial intensity variations and self-focusing also contribute to fluorescence signals that deviate from the usual single-atom saturation behavior.

DOI
10.1103/physreva.28.238

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John Huennekens, Alan Gallagher

We have measured cross sections, ${\ensuremath{\sigma}}_{\mathrm{nL}}$, for the excitation transfer process $\mathrm{Na}(3P)+\mathrm{Na}(3P)\ensuremath{\rightarrow}\mathrm{Na}(3S)+\mathrm{Na}(\mathrm{nL})$, where $\mathrm{nL}$ is the $4D$ or $5S$ level. Our results are ${\ensuremath{\sigma}}_{4D}=23 {\AA{}}^{2}\ifmmode\pm\else\textpm\fi{}35%$ and ${\ensuremath{\sigma}}_{5S}=16 {\AA{}}^{2}\ifmmode\pm\else\textpm\fi{}35%$ at $T\ensuremath{\sim}600$ K. To obtain these cross sections we have used pulsed excitation and measured the intensities of $4D$, $5S$, and $3P$ fluorescence emissions, and the spatial distribution of excited atoms resulting from radiation diffusion, as well as the excited atom density as a function of time. Additionally, we have accounted for (time-dependent) radiation trapping of $3P$ and $\mathrm{nL}$ level radiation and for the resulting anisotropies of these fluorescence emissions. Comparisons of our results with theory have been made, and their relevance to other experiments is discussed.

Physical Review A•Feb 1, 1983•74 citations
We have measured the time-dependent fluorescence of the sodium DDD lines following pulsed excitation of one DDD line, in the presence of radiation trapping with optical depths k0L{k}_{0}Lk0​L of \ensuremath{\sim}10 to 2000. When collisional coupling of the 3P123{P}_{\frac{1}{2}}3P21​​ and 3P323{P}_{\frac{3}{2}}3P23​​ levels and different radiative-escape probabilities for each DDD line are taken into account, we obtain excellent agreement with Holstein's theory for the effective radiative decay rates in the Doppler region (k0L\ensuremath∼10\ensuremath−300{k}_{0}L\ensuremath{\sim}10\ensuremath{-}300k0​L\ensuremath∼10\ensuremath−300) and in the redistributed Lorentzian region (k0L>1000{k}_{0}L>1000k0​L>1000). For k0L{k}_{0}Lk0​L between these two regions, we observe an abrupt transition between the two limiting formulas. The buildup rate of the sensitized fluorescence signal also yields a 3P32\ensuremath→3P123{P}_{\frac{3}{2}}\ensuremath{\rightarrow}3{P}_{\frac{1}{2}}3P23​​\ensuremath→3P21​​ excitation transfer cross section in agreement with our previously reported cw measurement. Additionally, we have measured the dependence of the 3P3P3P fluorescence on laser power and beam diameter, and we explain the observed approach to saturation. We suggest that the previously reported "anomalous" approaches to saturation may be explained in terms of the laser beam burning through the optically thick vapor. Laser-beam spatial intensity variations and self-focusing also contribute to fluorescence signals that deviate from the usual single-atom saturation behavior.
Sodium vapor, in the density range 1013{10}^{13}1013 to 5 \ifmmode\times\else\texttimes\fi{} 1014{10}^{14}1014 ${\mathrm{cm}}^{\ensuremath{-}3}$, was excited by a cw dye laser, tuned 20-150 GHz from either the D1{D}_{1}D1​ or D2{D}_{2}D2​ resonance line. We observed a three-peak scattered spectrum, consisting of the Rayleigh component at the laser frequency, and the two fluorescence components (direct and sensitized) at the atomic resonance-line frequencies. Corrections to the Rayleigh signals for anisotropy and polarization effects, and to the fluorescence signals for radiation trapping, were made in order to obtain the ratio of the sum of the total intensities of the two fluorescence components to that of the Rayleigh component. This ratio combined with a measurement of the line-wing absorption coefficient yields the sodium density and the DDD-line self-broadening rate coefficients [${k}_{\mathrm{br}}=4.67\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}$ cm3{\mathrm{cm}}^{3}cm3${\mathrm{s}}^{\ensuremath{-}1}$ (\ifmmode\pm\else\textpm\fi{}15%) for the D2{D}_{2}D2​ line and ${k}_{\mathrm{br}}=3.07\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}$ cm3{\mathrm{cm}}^{3}cm3${\mathrm{s}}^{\ensuremath{-}1}$ (\ifmmode\pm\else\textpm\fi{}15%) for the D1{D}_{1}D1​ line]. Asymmetry in the self-broadened line wings due to fine-structure recoupling was observed. The measured intensity ratio of the DDD lines, combined with pulsed measurements of the effective radiative decay rates in the presence of radiation trapping, yields the fine-structure collisional-mixing cross section [$\ensuremath{\sigma}(3{P}_{\frac{3}{2}}\ensuremath{\rightarrow}3{P}_{\frac{1}{2}})=172$A˚2{\mathrm{\AA{}}}^{2}A˚2(\ifmmode\pm\else\textpm\fi{}18%)] at $T\ensuremath{\cong}300\ifmmode^\circ\else\textdegree\fi{}$ C. Our results are compared to other experiments and to theory.
The dencity of sodium was determined from measurement of optical absorption of the resonance line. Sodium vapour, in the dencity 3×10~(11) to 1.2×10~(12)cm~(-3), was excited by a cw dye laser, tuned 70 GHz from D_2 resonance line. We recorded signal intensities, consisting of The Rayleigh component at the laser frequency and the two fluorescence components (direct and sensitized) at the atomic resonance-line frequencies. D_2 line self-broadening rate coefficient [k_(br,2)=5.44×10~(-7)cm~3/s(±15%)] was yielded. Combined with the effective radiative decay rates in the presence of radiation trapping, we measured excitation-transfer rates in different dencities, for the excitation transfer process Na(3P_(3/2))+Na(3S) Na (3P_(1/2))+Na(3S). The fine-structure collisional-mining cross section [σ_(21)(3P_(3/2)→3P_(1/2))=19.9nm~2(±29%)3 at T 184℃ was obtained. Our results were compared to other experiments and to theory.
We present experiments of a laser with variable pulse energy and beam width saturating sodium vapor near the D1{D}_{1}D1​-line transition. At high optical depth and in a buffer gas atmosphere of argon, the effect of nonlinear radiation trapping is shown to drastically change the spatial distribution and temporal evolution of the excited-state population and of the fluorescence light trapped by the nonlinear medium. Besides observing the transient behavior of the fluorescence light, a pump-probe beam experiment enables us to gain a tomographic view inside the atomic vapor. Nitrogen as a buffer gas is used to compare with the situation where radiation trapping effects are negligible. Finally, numerical simulations based upon equations of radiative transfer for a two-level atomic system elucidate the role of nonlinear radiation trapping and support given interpretations of the experiments.
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.
We have measured cross sections, ${\ensuremath{\sigma}}_{\mathrm{nL}}$, for the excitation transfer process $\mathrm{Na}(3P)+\mathrm{Na}(3P)\ensuremath{\rightarrow}\mathrm{Na}(3S)+\mathrm{Na}(\mathrm{nL})$, where nL\mathrm{nL}nL is the 4D4D4D or 5S5S5S level. Our results are ${\ensuremath{\sigma}}_{4D}=23 {\AA{}}^{2}\ifmmode\pm\else\textpm\fi{}35%$ and ${\ensuremath{\sigma}}_{5S}=16 {\AA{}}^{2}\ifmmode\pm\else\textpm\fi{}35%$ at $T\ensuremath{\sim}600$ K. To obtain these cross sections we have used pulsed excitation and measured the intensities of 4D4D4D, 5S5S5S, and 3P3P3P fluorescence emissions, and the spatial distribution of excited atoms resulting from radiation diffusion, as well as the excited atom density as a function of time. Additionally, we have accounted for (time-dependent) radiation trapping of 3P3P3P and nL\mathrm{nL}nL level radiation and for the resulting anisotropies of these fluorescence emissions. Comparisons of our results with theory have been made, and their relevance to other experiments is discussed.