Cited by 303Laser-Matter Interactions and ApplicationsAtomic and Molecular PhysicsAdvanced Chemical Physics Studies

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Reconstruction and control of a time-dependent two-electron wave packet

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Ott, Christian, Kaldun, Andreas, Argenti, Luca, Raith, Philipp, Meyer, Kristina, Laux, Martin, Zhang, Yizhu, Blättermann, Alexander, Hagstotz, Steffen, Ding, Thomas, Heck, Robert, Madroñero, Javier, Martín, Fernando, Pfeifer, Thomas·2014·Nature

DOI 10.1038/nature14026

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Abstract

The concerted motion of two or more bound electrons governs atomic and molecular non-equilibrium processes including chemical reactions, and hence there is much interest in developing a detailed understanding of such electron dynamics in the quantum regime. However, there is no exact solution for the quantum three-body problem, and as a result even the minimal system of two active electrons and a nucleus is analytically intractable. This makes experimental measurements of the dynamics of two bound and correlated electrons, as found in the helium atom, an attractive prospect. However, although the motion of single active electrons and holes has been observed with attosecond time resolution, comparable experiments on two-electron motion have so far remained out of reach. Here we show that a correlated two-electron wave packet can be reconstructed from a 1.2-femtosecond quantum beat among low-lying doubly excited states in helium. The beat appears in attosecond transient-absorption spectra measured with unprecedentedly high spectral resolution and in the presence of an intensity-tunable visible laser field. We tune the coupling between the two low-lying quantum states by adjusting the visible laser intensity, and use the Fano resonance as a phase-sensitive quantum interferometer to achieve coherent control of the two correlated electrons. Given the excellent agreement with large-scale quantum-mechanical calculations for the helium atom, we anticipate that multidimensional spectroscopy experiments of the type we report here will provide benchmark data for testing fundamental few-body quantum dynamics theory in more complex systems. They might also provide a route to the site-specific measurement and control of metastable electronic transition states that are at the heart of fundamental chemical reactions.

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Self-citation
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Authors: Ott, C., Kaldun, A., Argenti, L., Raith, P., Meyer, K., Laux, M., Zhang, Y., Blättermann, A., Hagstotz, S., Ding, T., Heck, R., Madroñero, J., Martín, F., & Pfeifer, T.
Affiliations: Max Planck Institute for Nuclear Physics (DE)
Universidad Autónoma de Madrid (ES)
Technical University of Munich (DE)
Heidelberg University (DE)
Corresponding author: Pfeifer, Thomas
ORCID: Ott, Christian
Kaldun, Andreas
Argenti, Luca
Raith, Philipp
Meyer, Kristina
Zhang, Yizhu
Hagstotz, Steffen
Ding, Thomas
Heck, Robert
Madroñero, Javier
Pfeifer, Thomas
Venue: Nature
Publisher: Springer Science and Business Media LLC
Published: 2014-12
Volume: 516
Issue: 7531
Pages: 374-378
ISSN: 0028-0836 (ISSN-L)
1476-4687
DOI: 10.1038/nature14026
OpenAlex: W2057758931
Semantic Scholar: 85a9fdb2023d6ad1b8ff4d91a521251943cb980c
Cited by: 303
References: 38
Citations by year: 2026: 17 · 2025: 15 · 2024: 16 · 2023: 14 · 2022: 21 · 2021: 30 · 2020: 27 · 2019: 21 · 2018: 38 · 2017: 36 · 2016: 45 · 2015: 22 · 2014: 1
FWCI: 17.24
Type: journal article
Language: en
Open access: green
hdl.handle.net
Licence: other-oa
www.springer.com/tdm (tdm)
Locations: Nature (publishedVersion)
PubMed (publishedVersion)
LA Referencia (Red Federada de Repositorios Institucionales de Publicaciones Científicas) (acceptedVersion, other-oa)
Tesis Doctorals en Xarxa (Consorci de Serveis Universitaris de Catalunya) (acceptedVersion)
RePEc: Research Papers in Economics (submittedVersion)
Hispana (submittedVersion)
MPG.PuRe (Max Planck Society) (submittedVersion)
Biblos-e Archivo (Universidad Autónoma de Madrid) (submittedVersion, public-domain)
Topics: Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Atomic and Molecular Physics
Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Advanced Chemical Physics Studies
Keywords: helium atom, doubly excited states, quantum beats, attosecond transient absorption spectroscopy, Fano resonance, quantum interference, coherent control, electron correlation, multidimensional spectroscopy, attosecond spectroscopy, few-cycle laser fields

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Reconstruction and control of a time-dependent two-electron wave packet

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