Quasiclassical trajectory study of the dynamics of the H+N2O reaction on a new potential energy surface

Abstract

A new ab initio potential energy surface ͑PES͒ for the HϩN 2 O→OHϩN 2 reaction has been constructed using the GROW package of Collins and co-workers. The ab initio calculations have been done using the Becke three-parameter nonlocal exchange functional with the nonlocal correlation of Lee, Yang, and Parr density functional theory. A detailed quasiclassical trajectory study of integral and differential cross sections, product rovibrational populations, and internal energy distributions on the new PES is presented. The theoretical integral cross sections as a function of collision energy are in qualitative agreement with the experimental measurements. A good correspondence is found between the calculated OH(vЈϭ0,1) rovibrational populations and the recent measurements of Brouard and co-workers at 1.48 eV collision energy. In particular, the calculated kinetic energy release distributions for state resolved OH(vЈ,NЈ) products predict a substantial fraction of total energy going into rotational excitation of the N 2 co-product, in good agreement with the experimental findings.

Reaction of the hydrogen atom with nitrous oxide in aqueous solution – pulse radiolysis and theoretical study

“…The reaction of the Hc atom with N 2 O has been modelled in vacuum and in aqueous solution. Although the potential energy surface of the reaction Hc + N 2 O in the gas phase was computed previously by various methods, 13,[25][26][27][28][29][30] to the best of our knowledge the reaction path in aqueous solution is studied here for the rst time. The density functional theory (DFT) calculation have been performed using GAUSSIAN 09W.…”

Quasiclassical trajectory study of the SiH4+H→SiH3+H2 reaction on a global ab initio potential energy surface

“…However, the exact 12-dimensional global quantum dynamics calculations are still unaffordable nowadays; alternatively, the quasiclassical trajectory ͑QCT͒ calculations 25,26 in full dimensionality are feasible. In fact, the QCT method has been widely used to study all kinds of dynamical problems for reaction systems involving three and four atoms [27][28][29][30][31][32][33][34][35][36][37][38][39][40][41][42][43] over the decades and is becoming popular in studying the reaction dynamics of larger systems. [44][45][46][47][48][49] In the present work, we performed detailed QCT calculations on the 12-dimensional ab initio WSB surface 22 for the SiH 4 +H→ SiH 3 +H 2 reaction.…”

Reaction rate of H atoms with N2O in hot water

“…It is interesting to compare the rate constant for reaction 3 in water with the gas phase high pressure limit. The gas phase mechanism and rate of reaction 3 has been studied for decades due to its importance in combustion processes [27][28][29][30] . Two reaction channels have been identified.…”