Radiationless decay spectrum of O 1s double core holes in liquid water
| Autor: | Trinter, Florian, Inhester, Ludger, Püttner, Ralph, Malerz, Sebastian, Thürmer, Stephan, Marchenko, Tatiana, Piancastelli, Maria Novella, Simon, Marc, Winter, Bernd, Hergenhahn, Uwe |
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| Rok vydání: | 2024 |
| Předmět: | |
| Zdroj: | J. Chem. Phys. 160, 194503 (2024) |
| Druh dokumentu: | Working Paper |
| DOI: | 10.1063/5.0205994 |
| Popis: | We present a combined experimental and theoretical investigation of the radiationless decay spectrum of an O 1s double core hole in liquid water. Our experiments were carried out using liquid-jet electron spectroscopy from cylindrical microjets of normal and deuterated water. The signal of the double-core-hole spectral fingerprints (hypersatellites) of liquid water is clearly identified, with an intensity ratio to Auger decay of singly charged O 1s of 0.0014(5). We observe a significant isotope effect between liquid H$_2$O and D$_2$O. For theoretical modeling, the Auger electron spectrum of the central water molecule in a water pentamer was calculated using an electronic-structure toolkit combined with molecular-dynamics simulations to capture the influence of molecular rearrangement within the ultrashort lifetime of the double core hole. We obtained the static and dynamic Auger spectra for H$_2$O, (H$_2$O)$_5$, D$_2$O, and (D$_2$O)$_5$, instantaneous Auger spectra at selected times after core-level ionization, and the symmetrized oxygen-hydrogen distance as a function of time after double core ionization for all four prototypical systems. We consider this observation of liquid-water double core holes as a new tool to study ultrafast nuclear dynamics. Comment: Main manuscript: 28 pages, 8 figures. Supplementary Material: 16 pages, 9 figures |
| Databáze: | arXiv |
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