Electron impact resonances of uracil in an aqueous environment from anion photoelectron imaging
Electron impact resonances of uracil in an aqueous environment from anion photoelectron imaging
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阴离子光电子成像水环境中尿嘧啶的电子撞击共振
DOI：
10.1088/1361-6455/acf353
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发表时间：
2023
期刊：
影响因子：
--
通讯作者：
Cooper G
中科院分区：
文献类型：
--
作者：
Cooper G
溶剂化对尿嘧啶U电子附着的影响，通过探测尿嘧啶自由基阴离子U-在气相水簇U-（H2 O）n中的电子共振，使用光子能量范围内的光电子成像进行了研究。具体地，π 3* 形状共振被详细探测，并且考虑了激发到该共振之后的光谱特征。提供了几种新的分析方法，以捕获共振对光电子发射的不同作用，这反过来又提供了对π 3* 共振的位置及其后续动力学的洞察。溶剂化对通过光电子发射观察到的每个动作的影响进行了研究，为n = 10。我们发现的行动，无论是他们相关的统计发射，提示自动分离，或光电子的角分布，都变得不太敏感的集群大小的增加，这表明它们的使用非常大的集群可能是有限的。此外，我们认为电子脱离阴离子之间的相关性，在实验中探测，和电子附着到中性。具体而言，他们通过重组能量的线性响应图片，我们展示了如何在这里开发的集群方法允许一个分解的总重组能量到分子内（与阴离子到中性几何形状的变化U）和分子间（与水化球的变化）的贡献。对于U在一个散装水环境中，我们发现，总重组能，λ <$1.2 eV，显示来自分子内和分子间变化的贡献相等。
The effect that solvation has on electron attachment to uracil, U, was studied by probing the electronic resonances of the uracil radical anion, U−, in gas-phase water clusters, U−(H 2 O) n, using photoelectron imaging across a range of photon energies. Specifically, the π 3* shape resonance was probed in detail and the spectral signatures following excitation to this resonance are considered. Several new methods for analysis are provided to capture the different actions of the resonance on the photoelectron emission, which in turn provide insight into the location of the π 3* resonance and its subsequent dynamics. The effect of solvation on each action observed through the photoelectron emission is studied for n⩽ 10. We find that the actions—be they related to statistical emission, prompt autodetachment, or the photoelectron angular distributions—all become less sensitive as the cluster size increases, suggesting that their use for very large clusters may be limited. Additionally, we consider the correlation between electron detachment from the anion, as probed in the experiments, and electron attachment to the neutral. Specifically, they are linked through the reorganisation energy in a linear response picture and we show how the cluster approach developed here allows one to decompose the total reorganisation energy into intramolecular (associated with the anion to neutral geometry change in U) and intermolecular (associated with the change in hydration sphere) contributions. For U in a bulk aqueous environment, we find that the total reorganisation energy, λ∼ 1.2 eV, shows equal contributions from both intra-and intermolecular changes.
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影响因子：
8.4
作者：
Bull JN;West CW;Verlet JRR
通讯作者：
Verlet JRR
微水合分子共振形成的理论研究。
DOI：
10.1063/1.4993941
发表时间：
2017
期刊：
The Journal of chemical physics
影响因子：
--
作者：
A. Sieradzka;J. Gorfinkiel
通讯作者：
J. Gorfinkiel
对甲苯醌阴离子簇中 π* 共振的动力学。
DOI：
10.1039/c7cp03628k
发表时间：
2017
期刊：
Physical chemistry chemical physics : PCCP
影响因子：
--
作者：
J. Bull;J. Verlet
通讯作者：
J. Verlet
影响因子：
2.9
作者：
Anstoter, Cate S.;DelloStritto, Mark;Matsika, Spiridoula
通讯作者：
Matsika, Spiridoula
影响因子：
2.9
作者：
Coe, JV
通讯作者：
Coe, JV