Plane wave packet formulation of atom-plus-diatom quantum reactive scattering

We recently, interpreted several-re active scattering experiments using a plane wave packet (PWP) formulation of quantum scattering theory [see, e.g., S. C. Althorpe, F. Fernandez-Alonso, B. D: Beam, J.D. Ayers, A.E. Pomerantz; R.N. Zare, and E. Wrede, Nature (London) 416, 67 (2002)]. This paper presents the first derivation of this formulation for atom-plus-diatom reactive scattering, and explains its relation, to conventional time-independent reactive scattering: We generalize recent. results for spherical-particle. scattering [S.C. Althorpe, Phys. Rev. A 69, 042702 (2004)] to atom-rigid-rotor scattering in the space-fixed frame, atom-rigid-rotor scattering in the body-fixed frame, and finally A+BC rearrangement scattering. The reactive scattering is initiated by a plane wave packet, describing the, A+BC reagents, in center-of-mass scattering coordinates, and is detected by projecting onto; a series of AC+B (or AB+C) plane Wave "probe" packets. The plane wave packets are localized at the closest distance from the scattering center at which the interaction potential can be neglected. The time evolution of the initial plane wave packet provides a clear visualization of the scattering into space of the reaction products. The projection onto the probe packets yields the time-independent, state-to-state scattering amplitude, and hence the differential cross section. We explain how best to implement the PWP approach in a numerical computation, and illustrate this with a detailed application to the H+D-2. reaction. (C) 2004 American Institute of Physics.