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Title: Photoassociation of atoms in ultracold collisions probed by wave-packet dynamics

Journal Article · · Physical Review A; (United States)
; ;  [1]
  1. Laboratoire de Photophysique Moleculaire, Batiment 213, Universite de Paris-Sud, 91405 Orsay Cedex (France) Department of Chemistry, H.C. Orsted Institute, 2100 Copenhagen O (Denmark) Laboratoire de Chimie Physique, 11 rue Pierre et Marie Curie, 75231 Paris Cedex 05 (France) National Institute of Standards and Technology, Gaithersburg, Maryland 20899 (United States)

Photoassociation in laser-assisted collisions of ultracold alkali atoms has been used recently to perform high-precision spectroscopy of very-long-range states. Rovibrational spectra close to the Na(3 [sup 2][ital S])+Na[sup *](3 [sup 2][ital P][sub 3/2]) dissociation limit have been obtained by monitoring an enhanced Na[sub 2][sup +] ion signal. We propose the use of pump-probe techniques to study the dynamics of the ionization process. At very large distances (typically 70 a.u.) two colliding Na atoms absorb a photon and form a coherent vibrational wave packet. We follow the packet in time and probe two possible mechanisms that are proposed to yield molecular ions: [ital photoionization], where the second photon is absorbed at a small internuclear distance [ital R] directly ionizing the molecule, and [ital associative] [ital ionization] with excitation at intermediate [ital R] to the nuclear continuum of a doubly excited state followed by a half collision and autoionization at small [ital R]. The latter event can also lead to dissociation of the complex. The two mechanisms lead to distinct differences in the ion signals as a function of delay time between the pump and the probe pulses. Estimates of the ion rates to be expected in actual pump-probe experiments are given, which tend to favor the autoionization mechanism as the dominant reaction path.

OSTI ID:
7094838
Journal Information:
Physical Review A; (United States), Vol. 50:6; ISSN 1050-2947
Country of Publication:
United States
Language:
English