The birth and evolution of solvated electrons in the water
| Autor: | Fabio Novelli, Kaixuan Chen, Adrian Buchmann, Thorsten Ockelmann, Claudius Hoberg, Teresa Head-Gordon, Martina Havenith |
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| Rok vydání: | 2023 |
| Předmět: | |
| Zdroj: | Proceedings of the National Academy of Sciences of the United States of America, vol 120, iss 8 |
| ISSN: | 1091-6490 0027-8424 |
| Popis: | The photo-induced radiolysis of water is an elementary reaction in biology and chemistry, forming solvated electrons, OH radicals, and hydronium cations on fast time scales. Here, we use an optical-pump terahertz-probe spectroscopy setup to trigger the photoionization of water molecules with optical laser pulses at ~400 nm and then time-resolve the transient solvent response with broadband terahertz (THz) fields with a ~90 fs time resolution. We observe three distinct spectral responses. The first is a positive broadband mode that can be attributed to an initial diffuse, delocalized electron with a radius of (22 ± 1) Å, which is short lived (−1 that is well reproduced by ab initio molecular dynamics. We interpret this negative band at 110 cm −1 as the solvent cage characterized by a weakening of the hydrogen bond network in the first and second hydration shells of the cavity occupied by the localized electron. |
| Databáze: | OpenAIRE |
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