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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Intramolecular Dynamics in the Photofragmentation of Initially Vibrationally Excited CH_2Cl_2
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Intramolecular Dynamics in the Photofragmentation of Initially Vibrationally Excited CH_2Cl_2

机译：最初振动激发的CH_2Cl_2光碎裂的分子内动力学

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摘要

The intramolecular dynamics of dichloromethane was studied by applying vibrationally mediated photodis-sociation and photoacoustic spectroscopy.The parent species were initially excited to the second,third,and fourth C-H stretch overtone regions and subsequently photodissociated by approx 235 nm photons that also tagged the ground,Cl(~2P_(3/2)) [Cl],and spin-orbit-excited,Cl(~2P_(1/2)) [Cl~*],state photofragments via resonantly enhanced multiphoton ionization.The Cl and Cl~* action spectra revealed enhancement of their yield as a result of rovibrational excitation with a C1~*/C1 ratio of about 1/2.The action and photoacoustic spectra manifested a multiple-peak structure,which in terms of normal- and local-mode models is shown to be related to overtones of C-H stretches or combination bands of C-H stretches and bends.The measured time-of-flight profiles together with the determined C1~*/C1 branching ratios suggest fast dissociation and involvement of upper states of A' and A" symmetry,mixing via curve crossing and releasing both Cl and Cl~*.The determined C1~*/C1 ratios in photodissociation of vibrationally excited CH_2C1_2 are higher than those obtained previously in 193 nm photodissociation of the vibrationless ground state,implying higher nonadiabaticity for the former.
机译：通过应用振动介导的光解离和光声光谱技术研究了二氯甲烷的分子内动力学。首先将母体物种激发到第二，第三和第四个CH拉伸泛音区域，然后被约235 nm的光子光解离，该光子也标记了地面， Cl（〜2P_（3/2））[Cl]，并自旋轨道激发，Cl（〜2P_（1/2））[Cl〜*]，通过共振增强的多光子电离态形成光碎片。 *动作光谱揭示了由于振动激发而产生的收率提高，C1〜* / C1比约为1/2。动作光谱和光声光谱表现出多峰结构，在正常模式和局部模式下模型显示与CH伸展的泛音或CH伸展和弯曲的组合带有关。测得的飞行时间剖面以及确定的C1〜* / C1分支比表明快速解离并涉及A'的上态和A“对称，m振动激发的CH_2C1_2的光解离中确定的C1〜* / C1比值高于无振动基态的193 nm光解离中获得的值，这意味着前者的非绝热性更高。

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