Time-Dependent Wave-Packet Quantum Dynamics Study of the Ne + D₂⁺ (v₀ = 0–2, j₀ = 0) → NeD⁺ + D Reaction: Including the Coriolis Coupling

Abstract

The dynamics of the Ne + D2(+) (v0 = 0-2, j0 = 0) → NeD(+) + D reaction has been investigated in detail by using an accurate time-dependent wave-packet method on the ground 1(2)A' potential energy surface. Comparisons between the Coriolis coupling results and the centrifugal-sudden ones reveal that Coriolis coupling effect can influence reaction dynamics of the NeD2(+) system. Integral cross sections have been evaluated for the Ne + D2(+) reaction and its isotopic variant Ne + H2(+), and a considerable intermolecular isotopic effect has been found. Also obvious is the great enhancement of the reactivity due to the reagent vibrational excitation. Besides, a comparison with previous theoretical results is also presented and discussed.

The validities of centrifugal sudden approximations in chemical reaction dynamics

“…For the latter three systems, the CS approximations overestimate the integral cross sections over a high‐energy range. Other previous studies of He + NeH + , Ne + , Ne + , H + HeH + , He + HeH + , H + + LiH, and H + + D 2 also showed that the CS approximations do not work well for these ion–molecule reactions. Therefore, the failure of the CS approximations for the ion–molecule systems, as we showed in this review article, further suggest that the CS approximations should be cautiously used in the quantum dynamics study of the ion–molecule collisions, which has been first revealed by Han and coworkers in their studies of the other ion–molecule collision systems of D + + H 2 , He + , H − + D 2 , and D − + H 2 , .…”

“…However, in the time‐dependent wave packet study of Bulut and coworkers for the Li + and its isotopic variants, it has been showed that the CS approximation can yield reliable cross section and rate constant for this reaction system. With their wave packet study on the Ne + , Zhang and coworkers illustrated that the CS approximation failed in generating integral cross sections especially at high collision energies. Petrongolo and coworkers applied the time‐dependent RWP method to study the H( 2 S) + HeH + reaction from cold to hyperthermal energies.…”

“…And most importantly, their state‐to‐state dynamical codes are developed to be implemented on Graphic Processing Unit (GPU), which has greatly improved the computational efficiency of the quantum state‐to‐state studies. Using the GPU codes of Han and coworkers as well as other state‐to‐state codes of Balint‐Kurti and coworkers, Althorpe and coworkers, and so forth, several studies have also been performed to examine the validities of the CS approximations at a quantum state‐to‐state level, and all these studies showed the importance of including Coriolis couplings for getting the correct state‐to‐state dynamical quantities. Furthermore, the Coriolis‐coupled parallel computing strategy that we introduced in this review article, has been utilized into the state‐to‐state RWP code developed by the research group of Balint‐Kurti, this also has greatly improved the computational efficiency in Coriolis‐coupling studies at a quantum state‐to‐state level.…”

H2+ MOLEKÜLÜNÜN DÖNME ENERJİLERİNİN Ne + H2+  NeH+ + H REAKSİYONU ÜZERİNDEKİ ETKİSİ

“…The final work on this reaction was the use of deuterium, the isotope of the hydrogen atom, to investigate isotope effects. This work CC and CS calculations were, total cross sections of Ne + H2 + and Ne + D2 + reactions were investigated by depending on initial vibrational states [9].…”