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Physical Review Letters

Particle Formation by Resonant Laser Light in Alkali-Metal Vapor

A. Tam, George Moe, W. Happer

Published Dec 15, 1975• 148 citations
Publisher

Abstract

Resonant laser light causes micron-sized particles to form in cesium vapor when a small amount of hydrogen gas is present in the vapor. The particles are identified as cesium-hydride crystals. This is the first observation of light-induced particle formation in metal vapors. The phenomenon has relevance to lasers and nonlinear optical devices based on dense alkali vapors, and it may also be of interest for laser isotope-separation schemes.

DOI
10.1103/physrevlett.35.1630

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A new method of laser radiation generation without population inversion in the red wing of the $$D_{1}$$ -line of alkali metal atoms under resonant absorption of broadband radiation of pump laser diodes at the $$D_{1}$$ transition is studied theoretically. The appearance of laser generation is caused by the fact that the probability of stimulated emission in the red wing of the spectral line exceeds the probability of absorption if homogeneous broadening due to interaction between active particles and the buffer gas significantly exceeds the natural broadening (under high pressures of the buffer gas). Analytical formulas representing the operation of a transversely diode-pumped alkali metal vapor laser are obtained. It is found that cesium atoms are the most promising object for observation of laser generation without population inversion in the red wing of the $$D_{1}$$ -line of alkali metal atoms. In a sufficiently long active medium (the length of the medium is 50 times its width), the efficiency of pumping radiation conversion into laser radiation can reach 57% at a buffer gas pressure of 5 atm, a pump diode radiation intensity of 5 kW/cm $${}^{2}$$ , and a half-width of its spectrum of 1 cm $${}^{-1}$$ . The laser radiation frequency can be tuned by several tens of cm $${}^{-1}$$ .

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Resonant laser light causes micron-sized particles to form in cesium vapor when a small amount of hydrogen gas is present in the vapor. The particles are identified as cesium-hydride crystals. This is the first observation of light-induced particle formation in metal vapors. The phenomenon has relevance to lasers and nonlinear optical devices based on dense alkali vapors, and it may also be of interest for laser isotope-separation schemes.
We have studied the loading of gaseous alkali-metal atoms into glass cells held at about 2 K by light-induced atom desorption (LIAD). In LIAD loading, the cell containing dense helium gas and a small amount of alkali metal is irradiated with cw laser light. This technique has two unique features to be investigated: alkali-metal atoms are desorbed, even by weak laser irradiation, from the cell walls not covered visibly with alkali metal, and loading efficiency is much higher below the superfluid transition temperature for the helium inside the cell than above this temperature. On the basis of extensive experimental studies for Rb presented in this paper, we give a consistent picture of the loading mechanism: alkali-metal atoms are optically desorbed from alkali-metal particles on the walls, then transported effectively into the cell volume by helium-gas flow produced by the continuous evaporation of the helium film, which is supplied by the superfluid-film flow on the walls from the bulk liquid helium at the bottom of the cell.
A new and unusual phenomenon which we call light narrowing is reported and discussed in this paper. We discovered this effect in dense, spin-polarized cesium vapor optically pumped with a cw blue dye laser beam tuned to the second resonance D1{D}_{1}D1​ line (4593 \AA{}). We observe a significant narrowing of the radio-frequency power-broadened magnetic resonance lines (linewidths narrow by as much as a factor of 2.5) when the intensity of the circularly polarized incident dye laser beam is increased by either focusing the beam or by the removal of attenuating filters from the focused beam. The magnetic resonance linewidths in spin-polarized cesium vapor were measured over a wide range of cesium number densities (5\ifmmode\times\else\texttimes\fi{}1012{10}^{12}1012 ${\mathrm{cm}}^{\ensuremath{-}3}$ \ensuremath{\le}[Cs]\ensuremath{\le}1\ifmmode\times\else\texttimes\fi{}1016{10}^{16}1016 ${\mathrm{cm}}^{\ensuremath{-}3}$). This corresponds to cesium spinexchange rates of 4.5\ifmmode\times\else\texttimes\fi{}103{10}^{3}103 to 9\ifmmode\times\else\texttimes\fi{}106{10}^{6}106 ${\mathrm{sec}}^{\ensuremath{-}1}$. For low cesium number densities (5\ifmmode\times\else\texttimes\fi{}1012{10}^{12}1012 [Cs]3\ifmmode\times\else\texttimes\fi{}1014{10}^{14}1014 ${\mathrm{cm}}^{\ensuremath{-}3}$) the light-narrowing effect is large (a factor of 2.5) and independent of [Cs]. In the region of 3\ifmmode\times\else\texttimes\fi{}1014{10}^{14}1014 to 1\ifmmode\times\else\texttimes\fi{}1015{10}^{15}1015 ${\mathrm{cm}}^{\ensuremath{-}3}$ in number densities, the light-narrowing effect decreases with increasing [Cs]. At high cesium number densities ([Cs]> 1\ifmmode\times\else\texttimes\fi{}1015{10}^{15}1015 ${\mathrm{cm}}^{\ensuremath{-}3}$) this light-narrowing effect almost completely disappears. In the limit of low-radio-frequency power the magnetic resonance linewidths for focused and unfocused dye laser beam are nearly the same. Experimental observations on this new effect are presented in detail. In the latter part of this paper a self-contained theoretical treatment of the light-narrowing effect is developed. Using Bloch equations in the presence of optical pumping, spin relaxation (diffusion, electron randomization), rapid spin exchange, and radio-frequency magnetic field, expressions for magnetic resonance line shapes are derived. In general, we find good agreement between our experimental results and the theory.
We consider a gas of two-level atoms of two species (for example, natural Rb vapor consisting of two isotopes) in the field of laser radiation tuned close to resonance with the certain transition of a specific iostope. This radiation may turn to be rather close to a near lying transition of other isotope (within the linewidth of laser radiation), so it is necessary to take into account the possibility of excitation of other isotope in order to evaluate the enrichment degree if it is aimed at the isotope separation by means of selective excitation with subsequent chemcial reaction (in our example the rubidium hydride formation) of the excited isotope which is believed to take place at a rate much higher than that in the ground state of the atom.
Laser Generation without Population Inversion in the Red Wing of the D1{D}_{1}D1​-Line of Alkali Metal Atoms under Resonant Diode Pumping
A new method of laser radiation generation without population inversion in the red wing of the D1D_{1}D1​ -line of alkali metal atoms under resonant absorption of broadband radiation of pump laser diodes at the D1D_{1}D1​ transition is studied theoretically. The appearance of laser generation is caused by the fact that the probability of stimulated emission in the red wing of the spectral line exceeds the probability of absorption if homogeneous broadening due to interaction between active particles and the buffer gas significantly exceeds the natural broadening (under high pressures of the buffer gas). Analytical formulas representing the operation of a transversely diode-pumped alkali metal vapor laser are obtained. It is found that cesium atoms are the most promising object for observation of laser generation without population inversion in the red wing of the D1D_{1}D1​ -line of alkali metal atoms. In a sufficiently long active medium (the length of the medium is 50 times its width), the efficiency of pumping radiation conversion into laser radiation can reach 57% at a buffer gas pressure of 5 atm, a pump diode radiation intensity of 5 kW/cm 2{}^{2}2 , and a half-width of its spectrum of 1 cm −1{}^{-1}−1 . The laser radiation frequency can be tuned by several tens of cm −1{}^{-1}−1 .