Bond Order Potentials for a priori Simulations of Polyatomic Reactions

A Full Dimensional Quasiclassical Trajectory Study of Cl + CH4 Rate Coefficients

“…The main difference is found in the imaginary frequency value that is underestimated in the MEP-MPE PES. All the other details of this first MEP-MPE PES are given in refs and .…”

“…To obtain a better reproduction of the measured rate coefficients using a full dimensional QCT approach we investigated the possibility of building a new PES (the already mentioned MEP-MPE, Minimum Energy Path -Many Process Expansion PES 27,29 ) inspired to the scheme proposed by Ochoa and Clary 30 who generalized to polyatomic reactions the concept of many process expansion (MPE) approaches. 31-37…”

“…Accordingly, this paper is organized as follows: In Section 2 the results of a QCT study performed on the CTE PES are illustrated. In Section 3 a new potential energy surface of the Minimum Energy Path -Many Process Expansion (MEP-MPE) type 27 based on Bond Order (BO) coordinates is proposed, and the results of a QCT study performed on it are discussed. In Section 4, the kinetic isotopic effect obtained by substituting CH 4 with CD 4 is analyzed for both the CTE and the MEP-MPE PESs.…”

Collisional O2+ N2State-Selected Cross Sections for Open Science Cloud Reuse

“…These concepts are then applied in the paper to the MN PES to the end of modeling the energy dependence of the detailed cross sections computed on it for the O 2 + N 2 dissociative processes. The approach used for that purpose is the so-called many process expansion (MPE) BO representation in which the PES is formulated as a combination of process-specific BO channels connecting the reactants to the relevant products. − The coefficients of the combination allow a flexible switching among the process-specific terms while the formulation of the individual terms allows the accurate reproduction of local features.…”

MEP–MPE potential energy surface for the Cl + CH4 → HCl + CH3 reaction

“…To generalize the treatment to polyatomic reactions with more than four atoms, one needs to abandon the idea of including all processes and to follow each of them from the beginning to the end with a specific continuity variable. One can instead consider only those parts of the processes that are associated with one or more low‐energy minimum energy paths (MEPs) relevant to the key mechanisms of the overall process 19, 20.…”