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Multi-messenger tracking of coherence loss during bond breaking

arXiv
Authors: Tian Wang, Nida Haram, Zack Dube, Kyle A. Hamer, Yonghao Mi, Fatemeh Karimi, Andrei Yu. Naumov, Giulio Vampa, Caterina Vozzi, Xiaojun Liu, Albert Stolow, Michael Schuurman, Nicolas Douguet, David Villeneuve, Paul B. Corkum, Andre Staudte

Year

2025

Paper ID

5946

Status

Preprint

Abstract Read

~2 min

Abstract Words

146

Citations

N/A

Abstract

Coupled electronic and nuclear motions govern chemical reactions, yet disentangling their interplay during bond rupture remains challenging. Here we follow the light-induced fragmentation of Br2 using a coincidence-based multi-messenger approach. A UV pulse prepares the dissociative state, and strong-field ionization probes the evolving system. Coincident measurement of three-dimensional photoion and photoelectron momenta provides real-time access to both the instantaneous internuclear separation and the accompanying reorganization of the electronic structure, allowing us to determine the timescale of bond breaking. We find that electronic rearrangement concludes well before the nuclei reach the bond-breaking distance, revealing a hierarchy imposed by electron-nuclear coupling. Supported by semiclassical modelling, the results show that the stretched Br2 molecule behaves as a two-centre interferometer in which the loss of coherence between atomic centres encodes the coupled evolution of electrons and nuclei. Our work establishes a general framework for imaging ultrafast electron-nuclear dynamics in molecules.

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  • This paper contributes to the Quantum Chemistry research area in the Quantum Articles archive.
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  • Coupled electronic and nuclear motions govern chemical reactions, yet disentangling their interplay during bond rupture remains challenging.

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