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We thank M. Herve, E. Constant and G. Karras for fruitful discussions. All calculations were performed at the Centro de Computacion Cientifica (CCC) of the Universidad Autonoma de Madrid and the MareNostrum supercomputer of the Red Espanola de Supercomputacion. We acknowledge support from CNRS, ANR-16-CE30-0012 'Circe', ANR-15-CE30-0001 'CIMBAAD', the Federation de recherche Andre Marie Ampere 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 Innovacion (MICINN) project PID2019-105458RB-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 (CEX2020-001039-S) and the 'Maria de Maeztu' Programme for Units of Excellence in R&D (CEX2018-000805-M).

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Attosecond metrology of the two-dimensional charge distribution in molecules

Publicado en:Nature Physics. 20 (5): 765-769 - 2024-02-23 20(5), DOI: 10.1038/s41567-024-02406-2

Autores: Loriot, V; Boyer, A; Nandi, S; Gonzalez-Collado, C M; Plesiat, E; Marciniak, A; Garcia, C L; Hu, Y; Lara-Astiaso, M; Palacios, A; Decleva, P; Martin, F; Lepine, F

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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. Attosecond interferometry measurements of photoionization delays in planar carbon-based molecules can provide information on the dimension and shape of the two-dimensional hole generated in the process.

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