Photodissociation Dynamics of H2O and D2O via the D ̃ (1A1) Electronic State

Photodissociation Dynamics of H2O and D2O via the D ̃ (1A1) Electronic State
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通过 DÌ (1A1) 电子态研究 H2O 和 D2O 的光解离动力学

DOI:
10.1039/c9cp05321b
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发表时间:
2020
影响因子:
3.3
通讯作者:
Xueming Yang
Xueming Yang
中科院分区:
化学2区
文献类型:
--
作者:
Yao Chang;Jiami Zhou;Zijie Luo;Zhichao Chen;Zhigang He;Shengrui Yu;Li Che;Guorong Wu;Xingan Wang;Kaijun Yuan;Xueming Yang

文献摘要

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使用 H/D 原子里德堡标记飞行时间技术研究了 H2O 和 D2O 通过单光子激发态的光解离动力学。平行和垂直偏振下 H/D 原子产物的 TOF 光谱均已测量。产物平移能量分布和角度分布是从 TOF 光谱中得出的。通过模拟这些分布,确定了 OH/OD 乘积的量子态分布以及状态分辨角各向异性参数。 H2O/D2O 通过状态解离的最重要途径导致高度旋转激发的 OH/OD(X, v = 0) 产物,而 v ≥ 1 的振动激发的 OH/OD 产物仅占 OH/OD(X) 总数的三分之一。 OH(A)/OH(X)和OD(A)/OD(X)的支化比也已确定,H2O在122.12 nm处为1.0/3.0,D2O在121.95 nm处为1.0/2.2,这与先前理论预测的值相当一致。
Photodissociation dynamics of H2O and D2O via the state by one-photon excitation have been investigated using the H/D atom Rydberg tagging time-of-flight technique. The TOF spectra of the H/D-atom product in both parallel and perpendicular polarizations have been measured. Product translational energy distributions and angular distributions have been derived from TOF spectra. By simulating these distributions, quantum state distributions of the OH/OD product as well as the state-resolved angular anisotropy parameters were determined. The most important pathway of H2O/D2O dissociation via the state leads to highly rotationally excited OH/OD(X, v = 0) products, while vibrationally excited OH/OD products with v ≥ 1 comprise only one third of the total OH/OD(X) population. The branching ratios of OH(A)/OH(X) and OD(A)/OD(X) have also been determined, 1.0/3.0 for H2O at 122.12 nm and 1.0/2.2 for D2O at 121.95 nm, which are reasonably consistent with the values predicted by the previous theory.