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Chemical Physics Letters

Femtosecond crossed beam study of atom–atom collisions

R. Goldstein, Joachim Großer, O. Hoffmann, D. Wößner, G. Gerber, Hans-Juergen Schmidtke

Published Jul 1, 2002• 1 citation
Publisher
DOI
10.1016/s0009-2614(02)00927-2

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We report a measurement of the rate constant for associative ionization (AI) between excited Na(3p) atoms colliding within a single beam at a velocity of 11.9 ${\mathrm{msec}}^{\mathrm{\ensuremath{-}}1}$, corresponding to a temperature of 65 mK. The collisions take place in a narrow velocity class of excited atoms produced by crossing the collimated Na beam with a monomode dye laser at an angle of 45\ifmmode^\circ\else\textdegree\fi{}. Light polarized linearly in the collision plane yields an AI rate constant greater than that for circular polarization by a factor of 2. We find K65mKlin{K}_{65\mathrm{m}\mathrm{K}{}^{\mathrm{lin}}}K65mKlin​ =(12.2\ifmmode\pm\else\textpm\fi{}4.3)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}13}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{sec}}^{\mathrm{\ensuremath{-}}1}$ and K65mKcir{K}_{65\mathrm{m}\mathrm{K}{}^{\mathrm{cir}}}K65mKcir​ =(6.1\ifmmode\pm\else\textpm\fi{}1.8)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}13}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{sec}}^{\mathrm{\ensuremath{-}}1}$. The experimental arrangement also permits absolute calibration of earlier crossed-beam measurements of the excitation function (cross section versus velocity) at conventional thermal beam kinetic energies. Present results together with earlier work show that the cross-sectional temperature dependence is in qualitative accord with theory.
The pioneering works have demonstrated that the method of single collisions in crossed molecular beams is an important technique for achieving kinetic cool-ing of atoms or molecules in specific rotational states. In this study, we investigated the elastic and inelastic collisions between Al(2P1/2) metal atoms and O2 molecules at high collision energies in the range of 6.4–14.8 kcal/mol, utilizing the laser-ablation crossed beams in conjunction with time-sliced ion velocity map imaging tech-nique. We observed kinetic cooling of Al(2P1/2) atoms with an upper-limit laboratory-frame root-mean-square velocity of 24±3 m/s, corresponding to a translational temperature of 0.9±0.2 K in the laboratory frame, facilitated by the vibrational excitation of O2 (v′ = 1) in inelastic collisions. The translational cooling of Al atoms in the lab frame enhanced detection probability in the transformation of density-to-flux, as evidenced by the scattering images obtained during the experiments.