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Physical Review Letters

Observation of Structure in Laser-Induced Penning and Associative Ionization in Crossed-Beam Na + Na Collisions

Penelope Polak-Dingels, J. F. Delpech, J. Weiner

Published Jun 23, 1980• 64 citations
Publisher

Abstract

The results of double-laser experiments in which ${\mathrm{Na}}_{2}^{+}$ and ${\mathrm{Na}}^{+}$ are produced in crossed alkali beams under single-collision conditions in the presence of strong optical fields are reported. Structure in the mass-selected product ion intensity as a function laser frequency is observed when the optical field is strongly focused and tuned far off atomic or dimer transitions. These measurements are the first to show that the nuclear motion of the quasimolecular collision intermediate plays an important role in laser-induced collisional ionization.

DOI
10.1103/physrevlett.44.1663

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The results of double-laser experiments in which Na2+{\mathrm{Na}}_{2}^{+}Na2+​ and Na+{\mathrm{Na}}^{+}Na+ are produced in crossed alkali beams under single-collision conditions in the presence of strong optical fields are reported. Structure in the mass-selected product ion intensity as a function laser frequency is observed when the optical field is strongly focused and tuned far off atomic or dimer transitions. These measurements are the first to show that the nuclear motion of the quasimolecular collision intermediate plays an important role in laser-induced collisional ionization.
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.
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 report the direct observation of 6Li+^{6}\mathrm{Li}^{+}6Li+, 7Li+^{7}\mathrm{Li}^{+}7Li+, 13Li2+^{13}\mathrm{Li}_{2}^{+}13Li2+​, 14Li2+^{14}\mathrm{Li}_{2}^{+}14Li2+​ arising from single collisions between beams of lithium atoms in the presence of a laser field. Although the relative intensity of atomic ions reflects the natural isotopic abundance, a pronounced enrichment of 13Li2+^{13}\mathrm{Li}_{2}^{+}13Li2+​ relative to 14Li2+^{14}\mathrm{Li}_{2}^{+}14Li2+​ is observed.
For the first time, associative ionization has been observed in an atomic beam of excited sodium atoms in both the and the state. Relative values for the partial cross sections were obtained specified according to the different magnetic substate combinations of the two fine-structure states. These were found to be comparable to those for associative ionization between two atoms. However, the effect of the excitation on the ion production rate was found to be considerable and to depend strongly on the relative polarizations of the laser beams producing the two populations due to the redistribution of the involved magnetic sublevels. The results indicate that the initial orientation of the electron spin S does not significantly influence the associative ionization reaction at the mean collision energy of 25 meV.
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.