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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Ractive Quenchingof OH A ~2#SIGMA#~+ in Collisions with Molecualr Deuterium via Nonadiabatic passage through a Conical Intersection
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Ractive Quenchingof OH A ~2#SIGMA#~+ in Collisions with Molecualr Deuterium via Nonadiabatic passage through a Conical Intersection

机译：OH A〜2＃SIGMA＃〜+与分子氘碰撞通过非绝热通过圆锥形交叉点的猝灭

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摘要

The D and H atom products from collisional quenching of OH A ~2#SIGMA#~+ (v=0) by D_2 have been examined trough Doppler spectroscopy using two-photon (2 ~2S <-<- 1 ~2S) laser-induced fluorescence. A bimodal Doppler profile is observed for the d atoms, indicating that two different velocity distributions result from the OH A ~2#SIGMA#~+D_2->D+HOD reaction. Nearly 40% of the products are H atoms produced in the OH ~2#SIGMA#~++D_2->H+D_2O reaction with a single Gaussian profile. The two components of the D atom kinetic energy distribution are characterized by translational temperatures of approximately 1200 and 100000 K and on average account for 4% and 30% of the available energy. The H atom products accommodate about 37% of the available energy and are described by a 13000 K temperature. The translational energy distributions of the H/D atom products are attributed to two dynamical pathways through the strong nonadiabatic coupling region at the HO-D_2 conical intersection. The narrow "cold" distribution of D atoms arises from an abstraction reaction in a dirct passage through the conical intersection region. The broad statistical distribution observed for both D and H atom products suggests that the HO-D_2 collision pair lives long enough on the excitedstate surface for energy to randomize before evolving through the conical intersection that leads to products.
机译：使用双光子（2〜2S <-<-1〜2S）激光通过多普勒光谱法检查了D_2对OH A〜2＃SIGMA＃〜+（v = 0）的碰撞猝灭产生的D和H原子产物-诱导荧光。对于d原子观察到双峰多普勒分布，表明OH A〜2＃SIGMA＃〜+ D_2-> D + HOD反应产生两种不同的速度分布。接近40％的产物是OH〜2＃SIGMA＃〜++ D_2-> H + D_2O反应中具有单个高斯分布的H原子。 D原子动能分布的两个组成部分的特征是平移温度约为1200和100000 K，平均占可用能量的4％和30％。 H原子产物可容纳约37％的可用能量，并以13000 K的温度描述。 H / D原子产物的平移能量分布归因于通过HO-D_2圆锥形相交处的强非绝热偶合区域的两个动力学路径。 D原子的窄“冷”分布是由于通过圆锥形相交区域的直接通道中的抽象反应引起的。观察到的D和H原子产物的广泛统计分布表明，HO-D_2碰撞对在激发态表面上的寿命足够长，以使能量在经过形成产物的圆锥形相交之前随机化。

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