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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Photoelectron-Photofragment Coincidence Studies on the Dissociation Dynamics of the OH-CH4 Complex
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Photoelectron-Photofragment Coincidence Studies on the Dissociation Dynamics of the OH-CH4 Complex

机译：光电子 - 光折叠式巧合研究OH-CH4复合物的解离动力学

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摘要

Photoelectron photofragment coincidence (PPC) spectroscopy was used to characterize the energetics and dynamics of the OH + CH4 -> H2O + CH3 reaction initiated by photodetachment of the OH-(CH4) anion complex. PPC measurements at a photon energy of 3.20 eV yielded stable (OH-CH4 + e(-)) and dissociative (OH + CH4 (nu(1) or nu(3), v = 0, 1) + e(-)) channels. The main channel is dissociation to OH + CH4 + e(-) with a low kinetic energy release (KER), peaking at 0.04 eV. Interpretation of the experimental results was supported by quantum chemistry and quasiclassical trajectory calculations. The anion potential energy surface was constructed at the correlated coupled cluster singles, doubles, and perturbative triples level with augmented correlation consistent polarized valence triple-zeta basis set, and previously calculated neutral potential energy surfaces were used. Quasiclassical simulation of the dynamics of the OH-CH4 complex was carried out by selecting the momenta and coordinates from the Wigner distribution for the anion, providing the starting point for 4000 trajectories on the neutral potential energy surface. In agreement with the experimental results, most of the trajectories yield slowly recoiling OH + CH4 reactants while some are trapped in the entrance channel van der Waals well.
机译：光电子光折叠巧合（PPC）光谱法用于表征OH + CH 4 - > H 2 O + CH3反应的能量和动力学，通过光致张解的OH-（CH 4）阴离子复合物引发。 3.20 EV的光子能量的PPC测量产生稳定（OH-CH 4 + E（ - ））和分离（OH + CH 4（NU（1）或NU（3），V = 0,1）+ E（ - ））渠道。主通道与低动力能释放（KER）的低+ CH4 + E（ - ）解离，达到0.04eV。量子化学和拟痉挛轨迹计算支持实验结果的解释。阴离子电位能量表面在相关耦合的簇单打，加倍和扰动三元水平上构造，具有增强相关一致的极化价三Zeta基础组，并且使用先前计算的中性势能表面。通过从阴离子的Wigner分布中选择动矩和坐标来进行OH-CH4复合物的动态的拟CSICLICACE模拟，从而为中性势能表面提供4000个轨迹的起点。同意实验结果，大多数轨迹均慢慢重塑OH + CH4反应物，而一些则在入口通道范德沃尔斯陷阱。

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