Dynamical matching in a three-dimensional Caldera potential-energy surface.

In a previous paper, we used a recent extension of the periodic-orbit dividing surfaces method to distinguish the reactive and nonreactive parts in a three-dimensional (3D) Caldera potential-energy surface. Furthermore, we detected the phenomenon of dynamical matching in a 3D Caldera potential-energy surface. This happened for a specific value of the radius r of the periodic orbit dividing surfaces (r=0.25). In this paper, we demonstrated that the chemical ratios of the number of reactive and nonreactive trajectories to the total number of trajectories converges for a range of the radius r of the periodic-orbit dividing surfaces. This is important not only for validating the previous paper and to confirm that the method can detect the phenomenon of dynamical matching independently of the chosen radius of the construction of the dividing surface but also for investigating the application of the method to other Hamiltonian models.