High-Energy Reaction Dynamics of N_3
arxiv(2024)
摘要
The atom-exchange and atomization dissociation dynamics for the N(^4S) +
N_2(^1 Σ_ g^+) reaction is studied using a reproducing kernel
Hilbert space (RKHS)-based, global potential energy surface (PES) at the
MRCI-F12/aug-cc-pVTZ-F12 level of theory. For the atom exchange reaction (
N_A N_B + N_C→
N_A N_C + N_B), computed thermal rates and their temperature
dependence from quasi-classical trajectory (QCT) simulations agree to within
error bars with the available experiments. Companion QCT simulations using a
recently published CASPT2-based PES confirm these findings. For the atomization
reaction, leading to three N(^4
S) atoms, the computed rates from the RKHS-PES overestimate the
experimentally reported rates by one order of magnitude whereas those from the
PIP-PES agree favourably, and the T-dependence of both computations is
consistent with experiment. These differences can be traced back to the
different methods and basis sets used. The lifetime of the metastable N_3
molecule is estimated to be ∼ 200 fs depending on the initial state of the
reactants. Finally, neural network-based exhaustive state-to-distribution
models are presented using both PESs for the atom exchange reaction. These
models will be instrumental for a broader exploration of the reaction dynamics
of air.
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