权益分类	功能权益	普通用户	{{item.name}}会员
{{category.name}}	{{benefitItem.name}}

Ab initio quantum dynamics of photoabsorption and dissociation of carbon dioxide in the low lying singlet and triplet states

低位单重态和三重态二氧化碳光吸收和解离的从头算量子动力学

基本信息

批准号：
133201704
负责人：
Privatdozent Dr. Sergy Yu. Grebenshchikov
金额：
--
依托单位：
Chair of Theoretical and Computational Chemistry
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2009
资助国家：
德国
起止时间：
2008-12-31 至 2015-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/133201704?language=en
关键词：
Ab initio quantum dynamics photoabsorption

项目摘要

This project investigates the absorption spectrum and the dissociation dynamics of carbon dioxide in the ultraviolet (UV) wavelength range of 200 nm - 120 nm (6 eV - 10 eV). UV light destroys CO2 with unit quantum yield, and the chosen spectral region is of considerable importance for the atmospheric and planetary chemistry. The ab initio quantum dynamical studies of the six singlet states, performed in the first funding period, allowed a univocal electronic assignment of the principal absorption bands. Research in the second funding period concentrates on the six low lying triplet states and the photodynamic implications of their coupling with the singlet states. Extensive ab initio calculations of the coupled global potential energy, spin orbit, and the transition dipole moment surfaces are planned, followed by multistate quantum dynamical calculations. The goal of the project is to give a spectroscopically accurate description of the absorption properties of the coupled singlet and triplet manifolds and to elucidate the photodissociation mechanisms with the spatial, temporal, and energyresolution. The combined ab initio/quantum dynamical studies are desinged to rationalize a large body of experimental data and to investigate the impact of non-adiabatic and spin orbit interactions on the absorption spectra and the electronic, translational, vibrational, and angular distributions ofthe photofragments in the spin allowed and the spin forbidden dissociation channels.

本项目研究二氧化碳在200 nm - 120 nm（6 eV - 10 eV）紫外波长范围内的吸收光谱和解离动力学。紫外光以单位量子产率破坏CO2，并且所选择的光谱区域对于大气和行星化学相当重要。在第一个供资期间，对六个单重态进行了从头算量子动力学研究，对主要吸收带进行了明确的电子分配。第二个资助期的研究集中在六个低位三重态及其与单重态耦合的光动力学影响。广泛的从头计算耦合的全球势能，自旋轨道，和过渡偶极矩表面的计划，其次是多态量子动力学计算。该项目的目标是给出耦合单重态和三重态流形的吸收性质的光谱精确描述，并阐明具有空间，时间和能量分辨率的光解机制。结合从头算/量子动力学研究的目的是合理化的大量的实验数据和调查的影响，非绝热和自旋轨道相互作用的吸收光谱和电子，平移，振动和角分布的光碎片的自旋允许和自旋禁止的解离通道。