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355 nm Photodissociation of N2O3 Revealed by Velocity-Mapped Ion Imaging.
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2020-01-13 , DOI: 10.1021/acs.jpca.9b08688 Alex J Fairhall 1 , Mia M Orlando 1 , Jeffrey A Bartz 1
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2020-01-13 , DOI: 10.1021/acs.jpca.9b08688 Alex J Fairhall 1 , Mia M Orlando 1 , Jeffrey A Bartz 1
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Dinitrogen trioxide is proposed as a precursor to forming nitrous acid, an important source of hydroxyl radicals in the atmosphere. The spectroscopy and properties of N2O3 have been studied at high pressures or low temperatures, but there are no reports of its gas-phase photodissociation. This study investigates the 355 nm photodissociation of N2O3 in a DC-sliced velocity-mapped ion imaging apparatus using linearly polarized nanosecond pump and probe lasers. The N2O3 sample was generated by expanding NO and NO2 seeded in a He carrier gas. After photodissociation, a high fraction of the available energy ends up in translation of the products. Time-dependent density functional theory calculations confirm the parallel transition dipole assignment if the dissociation occurs from a nonplanar N2O3 conformation. The vector correlations are nearly at the physical limits for a system where μ||v⊥J. The DC-sliced velocity-mapped ion imaging technique is well-suited to investigate N2O3 photodissociation since it resolves product speeds and differentiates among the sources of NO+ in an expansion containing NO, NO2, HONO, and N2O3.
中文翻译：
速度映射离子成像揭示了355 nm N2O3的光解离。
三氧化二氮被提议作为形成亚硝酸的前体，亚硝酸是大气中羟基自由基的重要来源。已经在高压或低温下研究了N 2 O 3的光谱和性质，但是没有关于其气相光解离的报道。这项研究调查了使用线性偏振纳秒泵浦和探针激光器的直流切片速度映射离子成像设备中N2O3在355 nm的光解离。通过膨胀接种在He载气中的NO和NO2生成N2O3样品。光离解后，大部分可用能量最终转化为产物。如果解离发生于非平面的N2O3构象，则依赖于时间的密度泛函理论计算可确定平行跃迁偶极子分配。对于其中μ||v⊥J的系统，矢量相关性几乎处于物理极限。DC切片速度映射离子成像技术非常适合研究N2O3的光解离，因为它可以分解产物的速度并在包含NO，NO2，HONO和N2O3的膨胀中区分NO +的来源。
更新日期：2020-01-14
中文翻译：
速度映射离子成像揭示了355 nm N2O3的光解离。
三氧化二氮被提议作为形成亚硝酸的前体，亚硝酸是大气中羟基自由基的重要来源。已经在高压或低温下研究了N 2 O 3的光谱和性质，但是没有关于其气相光解离的报道。这项研究调查了使用线性偏振纳秒泵浦和探针激光器的直流切片速度映射离子成像设备中N2O3在355 nm的光解离。通过膨胀接种在He载气中的NO和NO2生成N2O3样品。光离解后，大部分可用能量最终转化为产物。如果解离发生于非平面的N2O3构象，则依赖于时间的密度泛函理论计算可确定平行跃迁偶极子分配。对于其中μ||v⊥J的系统，矢量相关性几乎处于物理极限。DC切片速度映射离子成像技术非常适合研究N2O3的光解离，因为它可以分解产物的速度并在包含NO，NO2，HONO和N2O3的膨胀中区分NO +的来源。
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