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An "inverse" harpoon mechanism.
- Source :
-
Science advances [Sci Adv] 2022 Sep 30; Vol. 8 (39), pp. eabq8084. Date of Electronic Publication: 2022 Sep 28. - Publication Year :
- 2022
-
Abstract
- Electron-transfer reactions are ubiquitous in chemistry and biology. The electrons' quantum nature allows their transfer across long distances. For example, in the well-known harpoon mechanism, electron transfer results in Coulombic attraction between initially neutral reactants, leading to a marked increase in the reaction rate. Here, we present a different mechanism in which electron transfer from a neutral reactant to a multiply charged cation results in strong repulsion that encodes the electron-transfer distance in the kinetic energy release. Three-dimensional coincidence imaging allows to identify such "inverse" harpoon products, predicted by nonadiabatic molecular dynamics simulations to occur between H <subscript>2</subscript> and HCOH <superscript>2+</superscript> following double ionization of isolated methanol molecules. These dynamics are experimentally initiated by single-photon double ionization with ultrafast extreme ultraviolet pulses, produced by high-order harmonic generation. A detailed comparison of measured and simulated data indicates that while the relative probability of long-range electron-transfer events is correctly predicted, theory overestimates the electron-transfer distance.
Details
- Language :
- English
- ISSN :
- 2375-2548
- Volume :
- 8
- Issue :
- 39
- Database :
- MEDLINE
- Journal :
- Science advances
- Publication Type :
- Academic Journal
- Accession number :
- 36170355
- Full Text :
- https://doi.org/10.1126/sciadv.abq8084