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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Photochemical Deactivation Process of HCFC-133a (C2H2F3CI): A Nonadiabatic Dynamics Study
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Photochemical Deactivation Process of HCFC-133a (C2H2F3CI): A Nonadiabatic Dynamics Study

机译：HCFC-133a（C2H2F3CI）的光化学失活过程：非绝热动力学研究

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摘要

The photochemical deactivation process of HCFC-133a (C2H2F3Cl) was investigated by computing excited-state properties with a number of single-reference methods, including coupled cluster to approximated second order (CC2), algebraic diagrammatic construction to second order (ADC(2)), and time-dependent density functional theory (TDDFT). Excited states calculated with these methods, especially TDDFT, show good agreement with our previous multireference configuration interaction (MR-CISD) results. All tested methods were able to correctly predict the properties of the main series of excited states, the n-sigma*, n-4p, and n-4s. Nonadiabatic dynamics in the gas phase considering 14 electronic states was simulated with TDDFT starting at the 10 +/- 0.25 eV spectral window, to be compared to experimental data measured after 123.6 nm excitation. The excited-state lifetime is 137 fs. Internal conversion to the ground state occurred through several different reaction pathways with different products, including atomic elimination (Cl, F, or H), multifragmentation mechanisms (Cl+F, Cl+H, or F+H), and CC bond-fission mechanisms (alone or with Cl or H elimination). The main photochemical channels observed were Cl, Cl+H, and Cl+F eliminations, representing 54% of all processes.
机译：HCFC-133a（C2H2F3Cl）的光化学失活过程通过使用多种单参考方法计算激发态性质进行了研究，包括将簇耦合至近似二阶（CC2），代数图解构建至二阶（ADC（2）） ），以及与时间有关的密度泛函理论（TDDFT）。用这些方法（尤其是TDDFT）计算出的激发态与我们以前的多参考配置相互作用（MR-CISD）结果显示出良好的一致性。所有测试的方法都能够正确预测主要激发态系列的性质，即n-sigma *，n-4p和n-4s。在10 +/- 0.25 eV光谱窗口处，以TDDFT模拟了考虑14种电子状态的气相非绝热动力学，并将其与123.6 nm激发后测得的实验数据进行比较。激发态寿命为137 fs。内部转化为基态的过程是通过几种具有不同产物的不同反应途径发生的，包括原子消除（Cl，F或H），多片段化机理（Cl + F，Cl + H或F + H）和CC键裂变机理（单独或消除Cl或H）。观察到的主要光化学通道为Cl，Cl + H和Cl + F消除，占所有过程的54％。

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