State- and time-resolved observation of ultrafast intermolecular proton transfer in hydrated biomolecules
Abstract Proton transfer underpins number of chemical and biochemical processes, yet its sub-100 fs dynamics have rarely been captured in real time. Here, we report direct and time-resolved observation of ionizing radiation-induced proton transfer in a heteroaromatic hydrate: the pyrrole-water compl...
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| Main Authors: | , , , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2025-07-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-61305-z |
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| Summary: | Abstract Proton transfer underpins number of chemical and biochemical processes, yet its sub-100 fs dynamics have rarely been captured in real time. Here, we report direct and time-resolved observation of ionizing radiation-induced proton transfer in a heteroaromatic hydrate: the pyrrole-water complex. Both the electron-impact and strong-field laser experiments create a locally and doubly charged pyrrole unit (C4H5N2+), which immediately (within 60 fs) donates a proton to the adjacent H2O, generating deprotonated C4H4N+ and hydronium H3O+ cations that subsequently undergo Coulomb explosion. The electron-impact experiments directly revealed initial states and provided dynamical insights through fragment ions and electron coincidence momentum imaging. The strong-field femtosecond laser experiments tracked the ultrafast dynamics of proton transfer; complementary ab initio calculations unraveled the dynamical details. The 50-60 fs proton transfer qualifies as one of the fastest acid-base reactions observed to date. This study offers a novel perspective on radiation-induced proton transfer in hydrated biomolecules. |
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| ISSN: | 2041-1723 |