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Vibronically and spin-orbit coupled diabatic potentials for X(2P) + CH4 → HX + CH3 reactions: Neural network potentials for X = Cl
Ist Teil von
The Journal of chemical physics, 2019-06, Vol.150 (24), p.244115-244115
Ort / Verlag
Melville: American Institute of Physics
Erscheinungsjahr
2019
Link zum Volltext
Quelle
AIP Journals Complete
Beschreibungen/Notizen
Vibronically and spin-orbit (SO) coupled diabatic potentials for the Cl(2P) + CH4 → HCl + CH3 reaction are constructed based on a recently developed approach [T. Lenzen and U. Manthe, J. Chem. Phys. 150, 064102 (2019)]. Diabatic potentials and couplings describing the entrance channel of the reaction are obtained based on ab initio data using a diabatization by an ansatz scheme. A detailed investigation of the electronic structure in the entrance channel using multireference configuration interaction (MRCI), coupled cluster [CCSD/CCSD(T)], and SO-MRCI calculations is presented. Neural networks using permutationally invariant polynomials as inputs are employed to represent the elements of the diabatic potential energy matrix. The same set of diabatic states is also used in the transition state region and all four exit channels. Here, the lowest adiabatic potential energy surface (PES) derived from the diabatic model is chosen to reproduce an adiabatic PES recently developed by Li and Guo. The accuracy of the resulting PES is evaluated, and the properties of the newly developed coupled diabatic potentials are analyzed in detail.