We report crossed beam experiments on the laser assisted collisions Na(3s) + M + hν f Na(3p) + M with M ) Kr, N 2 , and CO 2 . By varying the photon polarization, we gain direct insight into the geometric properties of the collision complex. For the Na + Kr system, we are able to deduce from the experimental data the two possible directions (Condon vectors) of the internuclear axis at the moment of the optical transition.

Experimental differential cross sections for the optical collision process K(4s) 2 S + Ar + hν → K(4p) 2 P + Ar are reported. The characteristic interference structures are used to determine the repulsive parts of the KAr X 2 and B 2 potential curves by comparison with the results of exact quantum coupled-channel scattering calculations. By a least-squares procedure we obtain potentials with a relative accuracy of typically 1% in the range 0 V 1000-1500 cm −1 , corresponding to absolute values of 2-4 cm −1 for the larger and 10-15 cm −1 for the smaller distances sampled by the experiment.

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New experimental results for the optical collision process Na(3s) + Kr + hν → Na(3p) + Kr are presented, which were obtained in a crossed-beam experiment with differential detection. The oscillatory structure in the differential cross-sections caused by Stueckelberg interferences is investigated in detail for relative velocities between 450 and 1500 m/s and for laser detunings Δν/c from 80 to 360 cm−1 on the blue-wing side of the Na resonance lines. The data are used to determine the potential of the excited repulsive B2Σ state of NaKr with an estimated accuracy of ±24 cm−1 (3 meV).