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Bulletin of the American Physical Society

Efficient collisional dissociation of Na{sub 2}{sup +} by laser-excited Na (3p)

Charles Tapalian, W. W. Smith

Published May 1, 1993• 0 citations
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Abstract

In studying ionization reactions in a single dense effusive beam of laser-excited Na(3p) atoms, we observe production of both Na{sub 2}{sup +} and Na{sup +} ions. The Na{sup +} results from the familiar associative ionization reaction of two Na(3p) atoms and the Na{sup +} ions under our conditions result mostly from the collisional dissociation of the Na{sub 2}{sup +} by reaction with a third excited Na(3p) atom, rather than from photo- dissociation or photoionization. A CW, single-frequency dye laser tuned to 589 nm resonantly excites the Na(3s) atoms to the 3p state. The atomic beam Na(3s) density is determined from low-intensity 589 absorption measurements. Na{sup +} ion yield depends on the cube of the Na beam density, suggesting successive collisions of three Na(3p) atoms: we believe the Na{sub 2}{sup +} ions polarize the third Na(3p) atom, resulting in a R{sup -4} orbiting collision interaction. A large collisional dissociation cross-section of approximately (4{plus_minus}2)x10{sup -13} cm{sup 2} results, for oven temperatures in the 500-600K range.

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•Feb 21, 1985•0 citations
In studying ionization reactions in a single dense effusive beam of laser-excited Na(3p) atoms, we observe production of both Na{sub 2}{sup +} and Na{sup +} ions. The Na{sup +} results from the familiar associative ionization reaction of two Na(3p) atoms and the Na{sup +} ions under our conditions result mostly from the collisional dissociation of the Na{sub 2}{sup +} by reaction with a third excited Na(3p) atom, rather than from photo- dissociation or photoionization. A CW, single-frequency dye laser tuned to 589 nm resonantly excites the Na(3s) atoms to the 3p state. The atomic beam Na(3s) density is determined from low-intensity 589 absorption measurements. Na{sup +} ion yield depends on the cube of the Na beam density, suggesting successive collisions of three Na(3p) atoms: we believe the Na{sub 2}{sup +} ions polarize the third Na(3p) atom, resulting in a R{sup -4} orbiting collision interaction. A large collisional dissociation cross-section of approximately (4{plus_minus}2)x10{sup -13} cm{sup 2} results, for oven temperatures in the 500-600K range.
We observe the production of Na2+ and Na+ arising from single collisions between crossed beams of sodium atoms when a laser field is tuned near the Na(3p 2P3/2) and Na(3p 2P1/2) transitions. Measurements of ion intensity vs laser intensity show that at moderately high power true laser-induced processes dominate over purely collisional effects. Relative intensity of mass-selected ions produced at either member of the Na resonance doublet shows conclusively that Na+ does not arise simply from photodissociation of Na2+ but must result from a direct, laser-induced collisional ionization.
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The authors report direct measurements of the photodissociation of Na 2 + ions created when a Na vapour in the density range 10 12 -10 13 cm -3 is irradiated by a pulsed laser with intensities in the 10 5 -10 6 W cm -2 range. The Na 2 + ions, accelerated by a weak electric field, are photodissociated in a second laser beam tuned to 6040 AA. In a preliminary experiment the Na 2 + ions are formed in the lowest vibrational levels and the measured photodissociation cross section is compared with existing calculations. When the Na vapour is irradiated at one of the 3S 1/2 -3P 1/2,3/2 resonances the photodissociation measurements show the existence of a distribution of rovibrational excited levels of the Na 2 + ions. A discussion is given in terms of associative ionisation in collisions of two Na(3p) atoms. The origin of the Na + ions produced simultaneously with the Na 2 + ions, in the vapour irradiated at resonance, is also discussed.
We report here measurements of two-body photoassociative ionization collisions between sodium atoms within an ultranarrow velocity class selected from a well-collimated, thermal atomic beam. Doppler-shifted excitation of the Na(3s2{\mathrm{}}^{2}2S1/2{\mathit{S}}_{1/2}S1/2​;F=1)\ensuremath{\rightarrow}Na(5p2{\mathrm{}}^{2}2P3/2{\mathit{P}}_{3/2}P3/2​) transition at 285 nm by a single-mode laser defines the narrow velocity class that subsequently populates the F=2 hyperfine level of the Na ground state by optical pumping. Probe laser beam excitation tuned near the Na(3s2{\mathrm{}}^{2}2S1/2{\mathit{S}}_{1/2}S1/2​;F=2)\ensuremath{\rightarrow}Na(3p2{\mathrm{}}^{2}2P3/2{\mathit{P}}_{3/2}P3/2​;F=3) transition produced photoassociative ionization with an average collision energy EK{\mathit{E}}_{\mathit{K}}EK​ corresponding to a temperature of 5.3 mK (EK{\mathit{E}}_{\mathit{K}}EK​=3/2kT). We determine the rate constant for the process as a function of probe beam intensity and polarization.
A summary of research performed under AFOSR Grant No. 83-0242 is given. The review describes molecular-beam studies of ion-pair production and measurements of the fraction of excited Na atoms, F*, in a composite beam of ground-state and excited Na atoms. Molecular beam techniques will be employed to study two-body reactions that will result in an intense, collimated beam of Li atoms at an energy of several hundred keV. Generating such a beam by charge transfer of a Li/sup +/ beam is not efficient at this energy. It appears that it can most efficiently be produced by forming a Li/sup -/ beam and stripping away valence electrons in a suitable gas. Plans are to study reactions associated with the production of Li/sup -/ beam which is formed when a Li/sup +/ beam interacts with a vapor of ground and excited (resonance state) Na atoms. One of the reactions (after Li/sup +/ has been converted to Li) is Li + Na yield Li/sup -/ + Na(+). This will be examined by merging a Li beam with a beam of Na atoms excited with a single frequency dye laser. The instrumentation required to complete this study consists of some laser and optical components,more » some vacuum equipment, and a laboratory computer system for data acquisition and analysis. This apparatus will supplement as well as rejuvenate an existing merging-beam apparatus.« less