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- W4386089682 abstract "Abstract The effect of solvation on electron attachment to uracil, U, was studied by probing the electronic resonances of the uracil radical anion, U–, in a gas-phase water clusters, U–(H2O)n, using photoelectron imaging at a range of photon energies. Specifically, the π3* shape resonance is probed in detail and the spectral signatures following excitation to this resonance are considered. Several new analysis methods are provided to capture the action of the resonance on the photoelectron emission, which in turn provide insight into the location of the π3* resonance and its subsequent dynamics. The effect of solvation on the action observed through the photoelectron emission is studied for n ≤ 10. We find that the action, 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. We additionally consider the correlation between electron detachment, as probed in the experiments, and electron attachment. 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) contributions. For U in a bulk aqueous environment, we find that the total reorganisation energy, λ ~ 1.2 eV, with equal contributions from both intra- and intermolecular changes.
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- W4386089682 created "2023-08-24" @default.
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- W4386089682 date "2023-08-23" @default.
- W4386089682 modified "2023-09-26" @default.
- W4386089682 title "Electron impact resonances of uracil in an aqueous environment from anion photoelectron imaging" @default.
- W4386089682 doi "https://doi.org/10.1088/1361-6455/acf353" @default.
- W4386089682 hasPublicationYear "2023" @default.
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