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Main Authors: Ngo, Loc Thi-Hoang, Codere, Julia, Ohara, Javin, Kaufman, Brian, Cohen, Martin G, Rozgonyi, Tamas, Marquetand, Philipp, Bain, Matthew, Pearson, Brett J, Forbes, Ruaridh, Weinacht, Thomas
Format: Preprint
Published: 2026
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Online Access:https://arxiv.org/abs/2605.03298
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author Ngo, Loc Thi-Hoang
Codere, Julia
Ohara, Javin
Kaufman, Brian
Cohen, Martin G
Rozgonyi, Tamas
Marquetand, Philipp
Bain, Matthew
Pearson, Brett J
Forbes, Ruaridh
Weinacht, Thomas
author_facet Ngo, Loc Thi-Hoang
Codere, Julia
Ohara, Javin
Kaufman, Brian
Cohen, Martin G
Rozgonyi, Tamas
Marquetand, Philipp
Bain, Matthew
Pearson, Brett J
Forbes, Ruaridh
Weinacht, Thomas
contents Tracking the coupled motion of electrons and nuclei on their intrinsic timescales is essential to understanding and controlling photochemical transformations. While attosecond techniques have provided unprecedented insight into electronic dynamics, they have largely been restricted to ionic systems, with nuclear motion often neglected or indirectly inferred. Here, we demonstrate a ``molecular attoscope", which uses shaped laser pulses in the deep ultraviolet to perform a coherent measurement of electronic and nuclear dynamics in an entangled wave packet in neutral benzene. This enables us to trace both the 856-attosecond-period electronic motion and the 36-femtosecond-period nuclear motion. We observe electronic coherence persisting over hundreds of optical cycles, modulated by nuclear dynamics. Our holographic approach is general, and lays the groundwork for coherent measurements capable of visualizing the evolution of the coupled electronic-nuclear wave function in real time.
format Preprint
id arxiv_https___arxiv_org_abs_2605_03298
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Molecular Attoscope: Pulse Shape Spectroscopy of Electronic Coherence
Ngo, Loc Thi-Hoang
Codere, Julia
Ohara, Javin
Kaufman, Brian
Cohen, Martin G
Rozgonyi, Tamas
Marquetand, Philipp
Bain, Matthew
Pearson, Brett J
Forbes, Ruaridh
Weinacht, Thomas
Quantum Physics
Tracking the coupled motion of electrons and nuclei on their intrinsic timescales is essential to understanding and controlling photochemical transformations. While attosecond techniques have provided unprecedented insight into electronic dynamics, they have largely been restricted to ionic systems, with nuclear motion often neglected or indirectly inferred. Here, we demonstrate a ``molecular attoscope", which uses shaped laser pulses in the deep ultraviolet to perform a coherent measurement of electronic and nuclear dynamics in an entangled wave packet in neutral benzene. This enables us to trace both the 856-attosecond-period electronic motion and the 36-femtosecond-period nuclear motion. We observe electronic coherence persisting over hundreds of optical cycles, modulated by nuclear dynamics. Our holographic approach is general, and lays the groundwork for coherent measurements capable of visualizing the evolution of the coupled electronic-nuclear wave function in real time.
title Molecular Attoscope: Pulse Shape Spectroscopy of Electronic Coherence
topic Quantum Physics
url https://arxiv.org/abs/2605.03298