Investigating the Rydberg States and Photodissociation Dynamics of Kr2 using Velocity Map Imaging

IF 1.1 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY
Cailum M K Stienstra, N. Coughlan, Alexander Haack, Patrick J. J. Carr, J. Crouse, Joshua Featherstone, Scott W. Hopkins
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引用次数: 0

Abstract

Although the krypton dimer, Kr2, is a prototypical weakly bound van der Waals complex in its ground electronic state, the excited states of Kr2 exhibit many and various interactions. Resonance enhanced multiphoton ionization and velocity map imaging provide an avenue to explore the electronic structure and photofragmentation dynamics of Kr2 in the vacuum ultraviolet region. By monitoring photofragmentation product channels and recoil anisotropy distributions, one can gain insights into excited state symmetries and lifetimes, which can aid in interpreting spectroscopy. Here, we study the spectroscopy and photodissociation dynamics of Kr2 in the 91,000 – 94,500 cm-1 region. We record and assign photofragment product channels for 32 vibronic bands corresponding to seven electronic transitions. We also identify two previously unobserved vibronic band systems, which we assign as the Kr2 5p [5/2]3 1g ← X0g+ and 5p [3/2]2 0g+ ← X0g+ transitions. Velocity map images show photofragments arising from predissociation of the neutral Rydberg states and from dissociative photoionization at the n > 2 photon level. We also observe variation in branching ratios between the predissociative and dissociative photoionization channels depending on the lifetime of the intermediate; longer lived states favour higher dissociative photoionization yields and exhibit β6 anisotropy parameters for predissociation product channels, indicating “rotational smearing” of the product angular distributions.
利用速度图成像技术研究Kr2的Rydberg态和光解动力学
虽然氪二聚体Kr2在基电子状态下是一个典型的弱束缚范德华配合物,但Kr2的激发态表现出许多不同的相互作用。共振增强多光子电离和速度图成像为探索真空紫外区Kr2的电子结构和光破碎动力学提供了一条途径。通过监测光破碎产物通道和反冲各向异性分布,人们可以深入了解激发态对称性和寿命,这有助于解释光谱。在这里,我们研究了Kr2在91,000 - 94,500 cm-1区域的光谱和光解动力学。我们记录并分配了对应于7个电子跃迁的32个振动带的光刻碎片产物通道。我们还确定了两个以前未观察到的振动带系统,我们将其命名为Kr2 5p [5/2]3 1g←X0g+和5p [3/2]2 0g+←X0g+跃迁。速度图图像显示了中性里德堡态的预解离和n > 2光子水平的解离光电离产生的光碎片。我们还观察到预解离和解离光电离通道之间分支比率的变化,这取决于中间体的寿命;较长的寿命态有利于较高的解离光电离产率,并且在预解离产物通道中表现出β6各向异性参数,表明产物角分布存在“旋转涂抹”。
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来源期刊
Canadian Journal of Chemistry
Canadian Journal of Chemistry 化学-化学综合
CiteScore
1.90
自引率
9.10%
发文量
99
审稿时长
1 months
期刊介绍: Published since 1929, the Canadian Journal of Chemistry reports current research findings in all branches of chemistry. It includes the traditional areas of analytical, inorganic, organic, and physical-theoretical chemistry and newer interdisciplinary areas such as materials science, spectroscopy, chemical physics, and biological, medicinal and environmental chemistry. Articles describing original research are welcomed.
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