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首页> 外文期刊>The Journal of Chemical Physics >Prompt release of O D-1 products upon UV excitation of CH2OO Criegee intermediates
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Prompt release of O D-1 products upon UV excitation of CH2OO Criegee intermediates

机译：在UV激励CH2OO Criegee中间体的紫外线激发时提示释放O D-1产品

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摘要

Velocity map imaging has been used to characterize the angular and velocity distributions of O D-1 photofragments arising from UV excitation of the simplest Criegee intermediate CH2OO in the long wavelength tail region (364 to 417 nm) of the B(1)A'-X(1)A' spectrum. The O D-1 images exhibit anisotropic angular distributions indicative of rapid dissociation to H2CO X(1)A(1) + O D-1 products, which occurs faster than the rotational period (ps) of CH2OO. As a result, the broad oscillatory structure reported previously in the longwavelength region of the UV absorption spectrum is attributed to short-lived resonances associated with the excited B(1)A' state of CH2OO, which decay by nonadiabatic coupling to repulsive singlet states. The total kinetic energy distributions show that nearly half of the available energy, on average, is partitioned to product translation. The balance results in significant internal excitation of the H2CO co-fragments. The product anisotropy and energy partitioning are unchanged across the UV spectrum and consistent with previously reported experimental and theoretical findings of the CH2OO B-X transition moment and dissociation energy to H2CO X(1)A(1) + O D-1 products. Published by AIP Publishing.
机译：速度映射成像已经用于表征来自B（1）A'-的长波长尾部区域（364至417nm）中的最简单的Criegee中间CH2OO的UV激发所产生的O D-1光ragragess的角速度分布。 x（1）频谱。 O D-1图像表现出直值角分布，其表明到H2CO X（1）A（1）+ O D-1产品的快速解离，其比CH2OO的旋转周期（PS）更快地发生。结果，在UV吸收光谱的长波长区域中报告的宽振荡结构归因于与激发的B（1）''的CH2OO状态相关的短寿命共振，其通过非驱散偶联与排斥单态衰减。总动能分布表明，近一半的可用能量平均地分配给产品翻译。平衡导致H2CO共碎片的显着内部激发。产品各向异性和能量分区在紫外谱中不变，并且与先前报道的CH2OO B-X转换片段和解离能的实验和理论发现一致至H2CO X（1）A（1）+ O D-1产品。通过AIP发布发布。

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