A DFT study of two-state reactivity on the reaction of N 2O with Sc + in the gas phase

Abstract

The mechanism of spin-forbidden reaction of N 2O (X 1∑) with Sc + has been systematically explored via density functional calculations in order to investigate the mechanisms of this reaction. Our calculated results strongly indicate that the pathway for N 2O and Sc + including several reaction pathways and numerous isomers, leads to oxidation, ScO + ( 1∑ +/ 3∑ +) + N 2 (X 1 ∑ g + ) or nitration, ScN + ( 2∑/ 4∑) + NO (X 2∏). Moreover, the attack of Sc + cation on oxygen atom in N 2O compound involves intersystem crossing (ISC) between singlet and triplet state potential energy surfaces (PESs). The crossing points (CPs) have been located by the intrinsic reaction coordinate (IRC) approach used by Yoshizawa et al., and corresponding minimum energy crossing points (MECPs) obtained by the mathematical algorithm proposed by Harvey et al. has also been used. Additionally, possible spin inversion processes are discussed using spin–orbit coupling (SOC) calculations.