Jiang Wenbin, Wang Xincheng, Zhang Shuai, Dong Ruichao, Guo Yuliang, Feng Jinze, Shen Zhenjie, Yan Tianmin, Zhu Zhiyuan, Jiang Yuhai
Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China.
Center for Transformative Science and School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China.
J Chem Phys. 2022 Aug 28;157(8):084302. doi: 10.1063/5.0102713.
Multi-ionization and subsequent Coulomb explosion (CE) of the NO molecule irradiated by a linearly polarized 800 nm laser field is investigated by a reaction microscope, where a number of CE channels of NO with q ≤ 5 for two-body fragmentation and q ≤ 8 for three-body fragmentation were observed. For two-body CE, by analyzing the internuclear separations extracted from kinetic energy releases (KERs), dissociation branching fractions, and laser intensity dependence, interestingly, we found that fragmentation NO → N + NO is produced directly from dissociating NO via non-sequential stairstep ionization, whereas most of the others result from the sequential stairstep ionization. For three-body CE, 25 fragmentation channels of NO (q = 3-8) are distinguished in the present charge-encoded multi-photoion coincidence plot, and the concerted fragmentation mechanism is nominated in a typical Dalitz plot. With the help of the numerical computation with the measured KERs and momentum correlation angles, the geometric structures of molecular ions prior to fragmentation are reconstructed, which display the bending motion and simultaneous two-bond stretching before the CE. Increasing of the bond length for high charged NO indicates the dominating stairstep ionization in the three-body fragmentation.
利用反应显微镜研究了线性偏振800nm激光场辐照下NO分子的多电离及随后的库仑爆炸(CE),观测到了两体碎裂时q≤5、三体碎裂时q≤8的多个NO的CE通道。对于两体CE,通过分析从动能释放(KER)中提取的核间距、解离分支比以及激光强度依赖性,有趣的是,我们发现碎裂NO→N + NO是通过非顺序阶梯电离直接从解离的NO产生的,而其他大多数情况则是由顺序阶梯电离导致的。对于三体CE,在当前电荷编码的多光子电离符合图中区分出了25个NO的碎裂通道(q = 3 - 8),并在典型的达利兹图中提出了协同碎裂机制。借助对测量的KER和动量相关角的数值计算,重建了碎裂前分子离子的几何结构,这些结构显示了CE前的弯曲运动和同时的双键拉伸。高电荷NO键长的增加表明三体碎裂中阶梯电离占主导。