Multi-messenger tracking of coherence loss during bond breaking

Fuente: arXiv
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Main Authors: Wang, Tian, Haram, Nida, Dube, Zack, Hamer, Kyle A., Mi, Yonghao, Karimi, Fatemeh, Naumov, Andrei Yu., Vampa, Giulio, Vozzi, Caterina, Liu, Xiaojun, Stolow, Albert, Schuurman, Michael, Douguet, Nicolas, Villeneuve, David, Corkum, Paul B., Staudte, Andre
Format: Preprint
Published: 2025
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author Wang, Tian
Haram, Nida
Dube, Zack
Hamer, Kyle A.
Mi, Yonghao
Karimi, Fatemeh
Naumov, Andrei Yu.
Vampa, Giulio
Vozzi, Caterina
Liu, Xiaojun
Stolow, Albert
Schuurman, Michael
Douguet, Nicolas
Villeneuve, David
Corkum, Paul B.
Staudte, Andre
author_facet Wang, Tian
Haram, Nida
Dube, Zack
Hamer, Kyle A.
Mi, Yonghao
Karimi, Fatemeh
Naumov, Andrei Yu.
Vampa, Giulio
Vozzi, Caterina
Liu, Xiaojun
Stolow, Albert
Schuurman, Michael
Douguet, Nicolas
Villeneuve, David
Corkum, Paul B.
Staudte, Andre
contents 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 Br$_2$ 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 Br$_2$ 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.
format Preprint
id arxiv_https___arxiv_org_abs_2512_16132
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Multi-messenger tracking of coherence loss during bond breaking
Wang, Tian
Haram, Nida
Dube, Zack
Hamer, Kyle A.
Mi, Yonghao
Karimi, Fatemeh
Naumov, Andrei Yu.
Vampa, Giulio
Vozzi, Caterina
Liu, Xiaojun
Stolow, Albert
Schuurman, Michael
Douguet, Nicolas
Villeneuve, David
Corkum, Paul B.
Staudte, Andre
Chemical Physics
Atomic Physics
Optics
Quantum Physics
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 Br$_2$ 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 Br$_2$ 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.
title Multi-messenger tracking of coherence loss during bond breaking
topic Chemical Physics
Atomic Physics
Optics
Quantum Physics
url https://arxiv.org/abs/2512.16132