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Optics Letters

Observation in a discharge of short-lived atomic states by intracavity absorption

Gilbert O. Brink, S. M. Heider

Published Aug 1, 1981• 7 citations
Publisher

Abstract

Optical absorption in short-lived excited states of atomic neon caused by dye-laser intracavity absorption has been observed. The states were excited by a microwave discharge in neon gas produced by a microwave cavity located inside the optical cavity of the dye laser. All transitions arising from the 2p manifold of states that are usually seen in emission are here seen in absorption. Best theoretical estimates of the number density of each of the 2p states in the discharge is about 10(5)-10(7)/cm(3), and the mean lifetime of the states is about 19 x 10(-9) sec.

DOI
10.1364/ol.6.000366

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Applied Optics•Feb 1, 1977•20 citations
Optical absorption in short-lived excited states of atomic neon caused by dye-laser intracavity absorption has been observed. The states were excited by a microwave discharge in neon gas produced by a microwave cavity located inside the optical cavity of the dye laser. All transitions arising from the 2p manifold of states that are usually seen in emission are here seen in absorption. Best theoretical estimates of the number density of each of the 2p states in the discharge is about 10(5)-10(7)/cm(3), and the mean lifetime of the states is about 19 x 10(-9) sec.
The interaction of polychromatic radiation of a dye laser with a neon gas-discharge plasma in shielded cylindrical tubes at medium gas pressures (1-30 Torr) near atomic spectral absorption lines of NeI atoms with wavelengths 650.6 and 656.2 nm was experimentally studied. Along the direction of propagation of the laser radiation, a shift in the central frequency of absorption is observed in the presence of inhomogeneities in the plasma column. The character of the optical transmission spectrum near narrow resonances was empirically shown to substantially depend on the density of absorbing atoms in a plasma; if this density exceeds 1012 cm-3, the contour of the transmission spectrum near the absorption resonance acquires a dispersive form. The general laws of the formation of nonstationary plasma transmission spectra depending on the laser power, the density of absorbing atoms, the nature of plasma inhomogeneities along the direction of propagation of laser radiation are examined in detail. The role of nonlinear and coherent effects and phase self-modulation during resonant interaction of short pulses of polychromatic laser radiation with gas-discharge plasma in narrow shielded tubes is discussed.
Theoretical quantitative considerations as well as experimental data are presented based on absorption population depletion coupled with cavity ringdown spectroscopy. The absorbing number densities inside the cavity are determined by numerical integration of the coupled rate equations. The number of photons involved in absorption, cavity losses due to mirror reflectivity and stimulated emission are taken into account. The principle is to monitor a first transition by cavity ringdown spectroscopy while a second transition, with a state in common, is resonantly excited by the decaying radiation of different frequency also trapped inside the optical cavity. A numerical example is given for atomic lines of neon and the measurements carried out in a supersonic slit-jet expansion discharge demonstrate the feasibility of the technique. The technique is also proven to work with two resonant transitions of C2. Translational velocity of the jet modifying the rate equations is included in the model.
The interaction of an intense optical-maser field with excited atoms in a gas discharge leads to a considerable change in the population of those levels which are resonant at the maser frequency. This will cause a change in the population of other levels that are connected to the maser levels through collision-induced nonradiative as well as radiative transitions. Using the 1.15-\ensuremath{\mu} optical maser, these effects have been studied in detail for the 2s2s2s levels of neon where the changes are completely due to collisions. By analyzing the intensity changes in spontaneous emission originating from a gas-discharge cell placed within the maser resonator, we have observed the approach to a partial thermalization of two closely spaced levels. In this way we have been able to obtain the atomic-collision cross section for excitation transfer between the 2s22{s}_{2}2s2​ and 2s32{s}_{3}2s3​ levels. In pure neon this has been found to be ${\ensuremath{\sigma}}_{23}=(2.3\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}$ cm2{\mathrm{cm}}^{2}cm2. For a helium-neon mixture the measured cross section is ${\ensuremath{\sigma}}_{23}=(1.8\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}$ cm2{\mathrm{cm}}^{2}cm2. The experimental method used to determine these cross sections eliminates the uncertainties caused by the effects of electron-atom collisions and radiative cascade. These techniques also yield the ratio of the Einstein coefficients for the transitions $2{s}_{2}\ensuremath{\rightarrow}2{p}_{10}$ and $2{s}_{3}\ensuremath{\rightarrow}2{p}_{10}$. The measured ratio is $\frac{{A}_{2}}{{A}_{3}}=3.0\ifmmode\pm\else\textpm\fi{}0.4$.
The spectral profile of the strongly resonance-broadened transition lambda 585.2 nm of Ne I has been studied in absorption. A narrow-band tunable dye laser probed a weak discharge in natural neon cooled with liquid nitrogen. The Lorentzian width extrapolated to zero density was found to be 108+or-20 MHz, consistent with the value 114+or-4 MHz calculated from the natural widths of the levels. There is no indication of the excess width found in earlier emission experiments in helium and neon. A preliminary result of (1.7+or-0.2)10 -21 MHz atom -1 m 3 was obtained for the broadening constant of lambda 585.2 nm in absorption at 77K. This is consistent with the value found in emission.
A new technique for quantitative detection of atomic absorption by intracavity dye-laser quenching is studied. For the sodium D(2) line, a sensitivity of 7 x 10(4) atoms/cm(3) x 1% quenching is obtained; and the sensitivity in single-pass detection is 4 x 10(8) atoms/cm(3) x 1% absorption for a 15-cm cell. Use of a cw dye laser improves the sensitivity and the stability. The dependence of the sensitivity on the bandwidth of laser action is measured, and a simple theoretical consideration is given for single-pass absorption.