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David Villeneuve

Publications and source records attributed to David Villeneuve.

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Multi-messenger tracking of coherence loss during bond breaking

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.

physics.chem-ph

Photon bunching in high-harmonic emission controlled by quantum light

Attosecond spectroscopy comprises several techniques to probe matter through electrons and photons. One frontier of attosecond methods is to reveal complex phenomena arising from quantum-mechanical correlations in the matter system, in the photon fields and among them. Recent theories have laid the groundwork for understanding how quantum-optical properties affect high-field photonics, such as strong-field ionization and acceleration of electrons in quantum-optical fields, and how entanglement between the field modes arises during the interaction. Here we demonstrate a new experimental approach that transduces some properties of a quantum-optical state through a strong-field nonlinearity. We perturb high-harmonic emission from a semiconductor with a bright squeezed vacuum field resulting in the emission of sidebands of the high-harmonics with super-Poissonian statistics, indicating that the emitted photons are bunched. Our results suggest that perturbing strong-field dynamics with quantum-optical states is a viable way to coherently control the generation of these states at short wavelengths, such as extreme ultraviolet or soft X-rays. Quantum correlations will be instrumental to advance attosecond spectroscopy and imaging beyond the classical limits.

quant-ph