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Reconstruction and control of a time-dependent two-electron wave packet
Open accessAbstract
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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“More recent experiments have addressed correlated two-electron dynamics [169], attosecond to few-femtosecond charge migration in molecules [170, 171] and electric field-induced charge separation in solids [172].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [169]
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Self-citationAzoury, D., Kruger, M. B., Orenstein, G., Larsson, H. R., Bauch, S., Bruner, B. D., & Dudovich, N. (2017) · Nature Communications · doi:10.1038/s41467-017-01723-w · Cited by 34
Ding, T., Rebholz, M., Aufleger, L., Hartmann, M., Meyer, K., Stooß, V., Magunia, A., Wachs, D., Birk, P., Mi, Y., et al. (2019) · Physical Review Letters · doi:10.1103/physrevlett.123.103001 · Cited by 30
Self-citationYang, Z. Q., Ye, D., Ding, T., Pfeifer, T., & Fu, L. (2015) · Physical Review A · doi:10.1103/physreva.91.013414 · Cited by 32
Self-citationAttosecond transient-absorption dynamics of xenon core-excited states in a strong driving field
Kobayashi, Y., Timmers, H. R., Sabbar, M., Leone, S. R., & Neumark, D. M. (2017) · Physical Review A · doi:10.1103/physreva.95.031401 · Cited by 29
Ryabikin, M. Y., Emelin, M. Y., & Strelkov, V. V. (2021) · Physics-Uspekhi · doi:10.3367/ufne.2021.10.039078 · Cited by 30
Attosecond science in atomic, molecular, and condensed matter physics
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Ayuso, D., Decleva, P., Patchkovskii, S., & Smirnova, O. V. (2018) · Journal of Physics B Atomic Molecular and Optical Physics · doi:10.1088/1361-6455/aabc95 · Cited by 27
Stooß, V., Hartmann, M., Birk, P., Borisova, G. D., Ding, T., Blättermann, A., Ott, C., & Pfeifer, T. (2019) · Review of Scientific Instruments · doi:10.1063/1.5091069 · Cited by 27
Self-citationAttosecond absorption and reflection spectroscopy of solids
Palo, N. D., Inzani, G., Dolso, G. L., Talarico, M., Bonetti, S., & Lucchini, M. (2024) · APL Photonics · doi:10.1063/5.0176656 · Cited by 29
Attosecond single-cycle undulator light: a review
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“Attosecond pulses have opened the possibilities to image [10] and control [11] the”
BackgroundRuberti, M. (2019) · Journal of Chemical Theory and Computation · doi:10.1021/acs.jctc.9b00288 · Cited by 26
Attosecond electronic dynamics of core-excited states of N2O in the soft x-ray region
Saito, N., Douguet, N., Sannohe, H., Ishii, N., Kanai, T., Wu, Y., Chew, A., Han, S., Schneider, B. I., Olsen, J., et al. (2021) · Physical Review Research · doi:10.1103/physrevresearch.3.043222 · Cited by 25
Self-citationKramers–Kronig relation in attosecond transient absorption spectroscopy
Leshchenko, V. E., Hageman, S. J., Cariker, C., Smith, G. P., Camper, A., Talbert, B. K., Agostini, P., Argenti, L., & DiMauro, L. F. (2022) · Optica · doi:10.1364/optica.474960 · Cited by 24
Self-citationAttosecond transient-absorption spectroscopy on aligned molecules
Bækhøj, J. E., & Madsen, L. B. (2016) · Physical Review A · doi:10.1103/physreva.94.043414 · Cited by 23
Nonlinear resonant Auger spectroscopy in CO using an x-ray pump-control scheme
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Ruberti, M. (2020) · Faraday Discussions · doi:10.1039/d0fd00104j · Cited by 23
Revealing Molecular Strong Field Autoionization Dynamics
Luo, S., Liu, J., Li, X., Zhang, D., Yu, X., Ren, D., Li, M., Yang, Y., Wang, Z., Ma, P., et al. (2021) · Physical Review Letters · doi:10.1103/physrevlett.126.103202 · Cited by 23
Signatures and control of strong-field dynamics in a complex system
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“In recent work, the phase of the dipole response after excitation was measured and controlled in a simple system, namely gaseous helium (31, 32).”
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Self-citationRebuilding the vibrational wavepacket in TRAS using attosecond X-ray pulses
Wang, C., Gong, M., Zhao, X., Nan, Q. W., Yu, X. Y., Cheng, Y., Kimberg, V., Liu, X.-J., Vendrell, O., Ueda, K., et al. (2024) · Communications Physics · doi:10.1038/s42005-023-01507-3 · Cited by 23
In situ characterization of few-cycle laser pulses in transient absorption spectroscopy
Blättermann, A., Ott, C., Kaldun, A., Ding, T., Stooß, V., Laux, M., Rebholz, M., & Pfeifer, T. (2015) · Optics Letters · doi:10.1364/ol.40.003464 · Cited by 22
Self-citationPotential Energy Surfaces of Core-Hole and Shake-Up States for Dissociative Ionization Studies
Corral, I., González‐Vázquez, J., & Martín, F. (2017) · Journal of Chemical Theory and Computation · doi:10.1021/acs.jctc.6b01214 · Cited by 22
Self-citationImpact of intense laser pulses on the autoionization dynamics of the 2s2p doubly excited state of He
Artemyev, A. N., Cederbaum, L. S., & Demekhin, P. V. (2017) · Physical Review A · doi:10.1103/physreva.96.033410 · Cited by 22
Perturbed ac Stark Effect for Attosecond Optical-Waveform Sampling
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Self-citation
Metadata
- 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
- Venue
- Nature
- Published
- 2014-12
- Volume
- 516
- Issue
- 7531
- Pages
- 374-378
- ISSN
- 0028-0836 (ISSN-L)
- 1476-4687
- 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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