Attochemical control of nuclear motion despite fast electronic decoherence
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arXiv
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| Natura: | Preprint |
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2025
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| _version_ | 1866918139365687296 |
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| author | Fransén, Lina Gomez, Sandra Vacher, Morgane |
| author_facet | Fransén, Lina Gomez, Sandra Vacher, Morgane |
| contents | Short-in-time, broad-in-energy attosecond or few-femtosecond pulses can excite coherent superpositions of several electronic states in molecules. This results in ultrafast charge oscillations known as charge migration. A key open question in the emerging field of attochemistry is whether these electron dynamics, which due to decoherence often last only for a few femtoseconds, can influence longer-time scale nuclear rearrangements. Herein, we address this question through full-dimensional quantum dynamics simulations of the coupled electron-nuclear dynamics initiated by ionization and coherent excitation of ethylene. The simulations of this prototype organic chromophore predict electronic coherences with half-lives of less than 1 fs. Despite their brevity, these electronic coherences induce vibrational coherences along the derivative coupling vectors that persist for at least 50 fs. These results suggest that short-lived electronic coherences can impart long-lasting legacies on nuclear motion, a finding of potential importance to the interpretation of attosecond experiments and the development of strategies for attochemical control. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2509_09345 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Attochemical control of nuclear motion despite fast electronic decoherence Fransén, Lina Gomez, Sandra Vacher, Morgane Chemical Physics Short-in-time, broad-in-energy attosecond or few-femtosecond pulses can excite coherent superpositions of several electronic states in molecules. This results in ultrafast charge oscillations known as charge migration. A key open question in the emerging field of attochemistry is whether these electron dynamics, which due to decoherence often last only for a few femtoseconds, can influence longer-time scale nuclear rearrangements. Herein, we address this question through full-dimensional quantum dynamics simulations of the coupled electron-nuclear dynamics initiated by ionization and coherent excitation of ethylene. The simulations of this prototype organic chromophore predict electronic coherences with half-lives of less than 1 fs. Despite their brevity, these electronic coherences induce vibrational coherences along the derivative coupling vectors that persist for at least 50 fs. These results suggest that short-lived electronic coherences can impart long-lasting legacies on nuclear motion, a finding of potential importance to the interpretation of attosecond experiments and the development of strategies for attochemical control. |
| title | Attochemical control of nuclear motion despite fast electronic decoherence |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2509.09345 |