Multidimensional reactive scattering with quantum trajectories: dynamics with 50-200 vibrational modes.
The dynamics of ensembles containing thousands of quantum trajectories are studied for multidimensional systems undergoing reactive scattering. The Hamiltonian and equations of motion are formulated in curvilinear reaction path coordinates, for the case of a planar (zero-torsion) reaction path. In order to enhance the computational efficiency, an improved least squares fitting procedure is introduced. This scheme involves contracted basis sets and the use of inner and outer stencils around points where fitting is performed. This method is applied to reactive systems with 50-200 harmonic vibrational modes which are coupled to motion along the reaction coordinate. Dynamical results, including trajectory evolution and time-dependent reaction probabilities, are presented and power law scaling of computation time with the number of vibrational modes is described.
Babyuk
Dmytro
D
Department of Chemistry and Biochemistry, Institute for Theoretical Chemistry, The University of Texas, Austin, Texas 78712, USA.
Wyatt
Robert E
RE