气相四原子反应的全维态-态量子动力学研究
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- 英文论文题名：State-to-state Differential Cross Sections for Four-Atom Reactions in full dimensions
- 论文作者：刘舒 ; 张东辉
- 英文论文作者：Shu Liu ; Dong H.Zhang ; Dalian Institute of Chemical Physics ; Chinese Academy of Sciences
- 年：2016
- 作者机构：中国科学院大连化学物理研究所分子反应动力学国家重点实验室;
- 论文关键词：态-态 ; 微分截面 ; 模式选择
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第十九分会：化学中的量子与经典动力学
- 语种：中文
- 分类号：O643.1
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第十九分会 ; 化学中的量子与经典动力学
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：206k
- 原文格式：D
- 会议级别：全国
摘要
态-态微分截面是实验可观测的极限,包括产物的全部量子态分辨信息,对我们认识化学反应有着极其重要的作用。在理论上精确计算出微分截面也是量子动力学研究的根本目标。我们用含时波包方法首次计算出H+H_2O→H_2+OH抽取反应初始基态、第一对称和反对称伸缩振动激发态的全维态-态微分截面。结果表明(100)和(001)态反应表现的非常相似,产生的OH仍然主要在振动基态,并且OH(v=1)的分布比例和基态与激发态的相对反应性非常接近,从而证实了局域模式图像。我们还首次计算出H+D_2O→D+HOD交换反应初始基态的全维微分截面。产物角分布在刚过阈值能量时表现出侧向散射,轨线分析表明这是交换反应过渡态的直接表现。并且散射角106度的微分截面随碰撞能量的变化在0.91和1.16eV处表现出两个明显的形貌共振结构。
The state-to-state Differential Cross Sections(DCSs) are the most detailed information that can be measured experimentally, and the ability to calculate them accurately has long been the goal of the theoretical dynamicist. We report the first full-dimensional state-to-state study for the H+H_2O→H_2+OH reaction with H_2O in the ground and the first symmetric and asymmetric stretching excited states. Our calculation revealed that the populations of OH in v=1 state from vibrational excited states are very close to the relative reactivity between the ground and vibrationally excited states, therefore verified the local mode picture for the reaction. We also extend the time-dependent wave-packet method to calculate the first full-dimensional state-to-state DCSs for the H+D_2O→D+HOD reaction with D_2O in the ground rovibrational state.
The state-to-state Differential Cross Sections(DCSs) are the most detailed information that can be measured experimentally, and the ability to calculate them accurately has long been the goal of the theoretical dynamicist. We report the first full-dimensional state-to-state study for the H+H_2O→H_2+OH reaction with H_2O in the ground and the first symmetric and asymmetric stretching excited states. Our calculation revealed that the populations of OH in v=1 state from vibrational excited states are very close to the relative reactivity between the ground and vibrationally excited states, therefore verified the local mode picture for the reaction. We also extend the time-dependent wave-packet method to calculate the first full-dimensional state-to-state DCSs for the H+D_2O→D+HOD reaction with D_2O in the ground rovibrational state.
引文
[1]Liu,S.;Zhang,D.H.Chem.Sci.2016,7:261.
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[3]Zhang,D.H.;Collins,M.A.;Lee,S.-Y.Science 2000,290:961.
[4]Fu,B.;Zhou,Y.;Zhang,D.H.Chem.Sci.2011,3:270.
[2]Bronikowski,M.J.;Simpson,W.R;Zare,R.N.J.Phys.Chem.1993,97:2204.
[3]Zhang,D.H.;Collins,M.A.;Lee,S.-Y.Science 2000,290:961.
[4]Fu,B.;Zhou,Y.;Zhang,D.H.Chem.Sci.2011,3:270.