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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Vibrationally Mediated Photodissociation of Ethylene Cation by Reflectron Multimass Velocity Map Imaging
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Vibrationally Mediated Photodissociation of Ethylene Cation by Reflectron Multimass Velocity Map Imaging

机译：Reflectron多质量速度图成像的振动介导的乙烯阳离子光解离

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摘要

A new imaging technique,reflectron multimass velocity map ion imaging,is used to study the vibrationally mediated photodissociation dynamics in the ethylene cation.The cation ground electronic state is prepared in specific vibrational levels by two-photon resonant,three-photon ionization via vibronic bands of (pi,nf) Rydberg states in the vicinity of the ionization potential of ethylene,then photodissociated through the (B ~2A_g) excited state.We simultaneously record spatially resolved images of parent C_2H_4~+ ions as well as photofragment C_2H_3~+ and C_2H_2~+ ions originating in dissociation from the vibronic excitations in two distinct bands,7/4_0~2 and 8/0_0~0,at roughly the same total energy.By analyzing the images,we directly obtain the total translation energy distributions for the two dissociation channels and the branching between them.The results show that there exist differences for competitive dissociation pathways between H and H_2 elimination from C_2H_4~+ depending on the vibronic preparation used,i.e.,on the vibrational excitation in the ground state of the cation prior to photodissociation.Our findings are discussed in terms of the possible influence of the torsional excitation on competition between direct dissociation,isomerization,and radiationless transitions through conical intersections among the numerous electronic states that participate in the dissociation.
机译：利用反射电子多质量速度图离子成像技术研究乙烯阳离子中的振动介导的光解离动力学。通过光子带的双光子共振，三光子电离，在特定的振动水平下制备阳离子基态电子态。 （pi，nf）Rydberg态在乙烯的电离势附近，然后通过（B〜2A_g）激发态进行光离解。我们同时记录了母体C_2H_4〜+离子以及光碎片C_2H_3〜+和C_2H_2〜+离子在大致相同的总能量下从两个不同的频带7 / 4_0〜2和8 / 0_0〜0的振动激发中解离而来，通过分析图像，我们直接获得了C_2H_2〜+离子的总平移能分布结果表明，从C_2H_4〜+消除H和H_2的竞争性离解途径存在差异，具体取决于所用的振动准备，即在光解离之前在阳离子基态下的振动激发。我们的发现是根据扭转激发对通过圆锥形交点进行的直接解离，异构化和无辐射跃迁之间的竞争的可能影响进行讨论的参与解离的众多电子州中。

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