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Physical Review A

Nonradiative transport of atomic excitation in Na vapor

Arthur Zajonc, A. V. Phelps

Published May 1, 1981• 30 citations
Publisher

Abstract

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 $3{P}_{\frac{1}{2},\frac{3}{2}}$ 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 $D1$ and $D2$ 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{}${10}^{20}$ 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.

DOI
10.1103/physreva.23.2479

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Journal of the Optical Society of America B•Nov 1, 2001•15 citations
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 m\ensuremath−3{\mathrm{m}}^{\ensuremath{-}3}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.
Experimental line profiles and integrated intensities for backscattered and forward-scattered resonance radiation using white-light excitation are compared with theory for Na densities between 1019{10}^{19}1019 and 1022{10}^{22}1022 atoms/m3{\mathrm{m}}^{3}m3. Absorption measurements are used to verify linewidth and line-wing asymmetry parameters and Na-vapor densities. The scattered spectral intensities are normalized to the incident flux using calibrated diffusers. Measurements of scattered intensities were also made as N2{\mathrm{N}}_{2}N2​ was added to the Na. The line profiles and integrated intensities were calculated using a model which assumes complete redistribution of the radiation scattered by an atom and takes into account both radiative and nonradiative transport of the resonance excitation. The theory includes the effects of quenching by Na2{\mathrm{Na}}_{2}Na2​ and by admixed N2{\mathrm{N}}_{2}N2​. With the white-light excitation used in these experiments the radiative transport is found to dominate the nonradiative transport except at wavelengths very near line center. The agreement between experimental and theoretical line profiles is good at high sodium densities (\ensuremath{\sim} 5 \ifmmode\times\else\texttimes\fi{} 1021{10}^{21}1021 atoms/m3{\mathrm{m}}^{3}m3) where instrumental resolution is not a serious limitation. The agreement between experimental and theoretical integrated intensities is within experimental error for Na densities of (1-10) \ifmmode\times\else\texttimes\fi{} 1019{10}^{19}1019 and (2-5) \ifmmode\times\else\texttimes\fi{} 1021{10}^{21}1021 atoms/m3{\mathrm{m}}^{3}m3. At the intermediate densities the approximately 20% discrepancy may be caused by the incomplete redistribution of radiation in the scattering process.
We have experimentally studied the nonradiative transport of excitation in a dense [N[N[N=(0.3-2.5)\ifmmode\times\else\texttimes\fi{}${10}^{17}{\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}]$ potassium vapor. We show that in such a high-density vapor the diffusive nonradiative transport of excitation via ``hopping'' of excitation in dipole-dipole collisions between excited- and ground-state atoms is dominant over the radiative transport through photons. The nonradiative transport mechanism becomes visible in the fluorescence-excitation spectrum signal as a sharp dip close to the resonance frequency. The appearance of the dip, its shape, width, and density dependence can all be explained in terms of a simple diffusion model for the nonradiative transport. This yields values for the diffusion coefficient and the resonance-exchange rate coefficient.
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.
Using a cw dye laser beam normally incident on a glass-Na-vapor interface, fluorescence excitation spectra of the D1{D}_{1}D1​ line are measured. By observing the fluorescence transmitted into the glass above the angle of total reflection, only evanescent light emitted within about a wavelength distance from the interface is observed. The measured spectra show a cutoff on the high-frequency side which is direct evidence for the transient behavior of the induced polarization of resonantly excited vapor atoms which have collided at the solid interface.
New experimental results and new phenomena related to the study of the retrofluorescence spectrum induced by a diode laser at the interface between glass and cesium vapor are presented. The Cs 62P3/2(Fe) hyperfine states are populated with a low-intensity tunable diode laser with a 10-MHz spectral bandwidth. We report an integrated atomic retrofluorescence spectrum in the 852.2-nm (62P3/2–62S1/2) resonance line and 917.2-nm (62D5/2–62P3/2) line generated by energy-pooling collisions. Emission spectra of the molecular fluorescence signal have been observed. At the resonance line a large proportion of the atoms excited by the laser are located in the vicinity of the surface. The interactions between the excited atomic 62P3/2 state and the surface appear as a spectral inhibition of the integrated retrofluorescence spectrum for both the atomic line and the molecular band. This spectral inhibition indicates that the nonradiative transformation process of changing atomically excited energy into thermal energy is preferred. We report the analysis of the dominant processes in the vicinity of the 852.2-nm resonance line, which can influence the retrofluorescence hyperfine spectrum at the boundary between the glass window and the saturated cesium vapor. Only the nonradiative transfer by evanescent waves toward the dissipative surface is retained. Using this mechanism, we formulate, for the first time to our knowledge, a simple model of a backscattered hyperfine fluorescence signal. The glass–vapor interface is considered as two distinct regions: a wavelength-thickness vapor layer joined to the surface and a more remote vapor region. The first region is analyzed as a spectral filter that annihilates the absorbed photons and the second one as a rich spectral light source. The experimental setup is described, and measured integrated retrofluorescence spectra are compared with predictions made by the model. The consistency between theory and experiment is remarkably good considering that the model depends only on two unknown parameters: the nonradiative transfer rate and the absorption shape line of the filtering region.