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Attosecond metrology of the two-dimensional charge distribution in molecules

Title: Attosecond metrology of the two-dimensional charge distribution in molecules
Authors: Loriot, V.; Boyer, A.; Nandi, S.; González-Collado, C. M.; Plésiat, E.; Marciniak, A.; García, C.L.; Hu, Y.; Lara-Astiaso, M.; Palacios Cañas, Alicia; Decleva, P.; Martín García, Fernando; Lépine, F.
Contributors: Facultad de Ciencias; Departamento de Química; Física Atómica y Molecular de Sistemas no Ligados (EXP C-052); Ab Initio Simulations of Electron-Nuclear Dynamics: from Atoms to Surfaces; Agencia Estatal de Investigación; Comunidad de Madrid
Publisher Information: Nature Research
Publication Year: 2026
Collection: Universidad Autónoma de Madrid (UAM): Biblos-e Archivo
Subject Terms: Molecules; time delay; attoseconds; carbon-based; molecular cations; Química
Description: Photoionization as a half-scattering process is not instantaneous. Usually, time delays in photoionization are on the order of tens of attoseconds. In going from a single atom to a nano-object, one can expect the delay to increase, since the photoelectron scatters over a larger distance. Here we show that this intuition is not correct when comparing three-dimensional and planar molecules. Using attosecond interferometry, we find that the time delays in two-dimensional (2D) carbon-based molecules can be significantly shorter than those of three-dimensional counterparts. The measured time delay carries the signature of the spatial distribution of the 2D hole created in the residual molecular cation, allowing us to obtain its dimensions with angstrom accuracy. Our results demonstrate that the photoionization delay depends on the symmetry and shape of the created hole, as we show by identifying a quadrupole contribution in the measured delay of 2D molecules ; We acknowledge support from CNRS, ANR-16-CE30-0012 ‘Circé’, ANR-15-CE30-0001 ‘CIMBAAD’, the Fédération de recherche André Marie Ampère and the European COST Action AttoChem (CA18222). C.M.G.C., E.P., A.P. and F.M. are supported by the Ministerio de Ciencia e Innovación (MICINN) project PID2019105458RB-I00 and the Comunidad de Madrid project FULMATEN (ref. Y2018NMT-5028). F.M. acknowledges support from the ‘Severo Ochoa’ Programme for Centres of Excellence in R&D (CEX2020001039-S) and the ‘Maria de Maeztu’ Programme for Units of Excellence in R&D (CEX2018-000805-M)
Document Type: article in journal/newspaper
File Description: application/pdf
Language: English
Relation: Nature Physics; https://doi.org/10.1038/s41567-024-02406-2; Gobierno de España. PID2019105458RB-I00; Gobierno de España. CEX2020001039-S; Gobierno de España. CEX2018-000805-M; Comunidad de Madrid. Y2018/NMT-5028/FULMATEN; https://hdl.handle.net/10486/736860; 765; 769; 20
DOI: 10.1038/s41567-024-02406-2
Availability: https://hdl.handle.net/10486/736860; https://doi.org/10.1038/s41567-024-02406-2
Rights: © The Author(s), under exclusive licence to Springer Nature Limited 2024 ; open access
Accession Number: edsbas.26FE3C7B
Database: BASE