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, attosecond to few-femtosecond charge migration in molecules, and electric field-induced charge separation in solids.
“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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“[16] assuming 2×10!! W/cm2 NIR-pump and 2×10!" W/cm2 NIR-probe intensities.”
Self-citationAttosecond transient absorption spectrum of argon at the L2,3 edge
Chew, A., Douguet, N., Cariker, C., Li, J., Lindroth, E., Ren, X., Yin, Y., Argenti, L., Hill, W. T., & Chang, Z. (2018) · Physical Review A · doi:10.1103/physreva.97.031407 · Cited by 50 · see citing works
Self-citationMultidimensional spectroscopy with attosecond extreme ultraviolet and shaped near-infrared pulses
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Some exact properties of the nonequilibrium response function for transient photoabsorption
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Callegari, C., Grum-Grzhimailo, A. N., Ishikawa, K. L., Prince, K. C., Sansone, G., & Ueda, K. (2021) · Physics Reports · doi:10.1016/j.physrep.2020.12.002 · Cited by 51 · see citing works
“…effect with synchrotron (Madden and Codling, 1963; Maeda et al., 1993; Sorensen et al., 1994; Domke et al., 1995, 1996) and attosecond XUV pulses (Ott et al., 2013, 2014; Kotur et al., 2016; Gruson et al., 2016; Cirelli et al., 2018) have been limited to the autoinizing states of neutral…”
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Nuclear-motion effects in attosecond transient-absorption spectroscopy of molecules
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Preparing attosecond coherences by strong-field ionization
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Barreau, L., Petersson, C. L. M., Klinker, M., Camper, A., Marante, C., Gorman, T. T., Kiesewetter, D., Argenti, L., Agostini, P., González‐Vázquez, J., et al. (2019) · Physical Review Letters · doi:10.1103/physrevlett.122.253203 · Cited by 42 · see citing works
Self-citationAdvances in high-order harmonic generation sources for time-resolved investigations
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“s shown in Fig. 5. The measured data (Fig. 5a) are in excellent agreement with the two-electron wave packet evolution simulated using either ab-initio TDSE calculations or a reduced model (Fig. 5b,c) [57]. From the comparison between the data and the theoretical expectation, it is possible to retrieve the relative pha…”
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Ultrafast quantum control of ionization dynamics in krypton
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Excited-state vibronic wave-packet dynamics in H 2 probed by XUV transient four-wave mixing
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Onset of ionic coherence and ultrafast charge dynamics in attosecond molecular ionisation
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“Attosecond spectroscopy based on single-photon absorption can provide valuable insight [1,2], albeit indirect, by following nonequilibrium electron dynamics in a time domain.”
Rabi oscillation in few-photon double ionization through doubly excited states
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Coherent Control of Photofragment Distributions Using Laser Phase Modulation in the Weak-Field Limit
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Symmetry of molecular Rydberg states revealed by XUV transient absorption spectroscopy
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Strong-field quantum control in the extreme ultraviolet domain using pulse shaping
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Dressing effects in the attosecond transient absorption spectra of doubly excited states in helium
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Self-citationAttosecond transient-absorption dynamics of xenon core-excited states in a strong driving field
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Attosecond science in atomic, molecular, and condensed matter physics
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Self-citationAttosecond absorption and reflection spectroscopy of solids
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Attosecond single-cycle undulator light: a review
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“Attosecond pulses have opened the possibilities to image [10] and control [11] the”
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Attosecond electronic dynamics of core-excited states of N2O in the soft x-ray region
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Self-citationKramers–Kronig relation in attosecond transient absorption spectroscopy
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Self-citationAttosecond transient-absorption spectroscopy on aligned molecules
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Nonlinear resonant Auger spectroscopy in CO using an x-ray pump-control scheme
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Revealing Molecular Strong Field Autoionization Dynamics
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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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Attosecond x-ray transient absorption spectroscopy in graphene
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Self-citationRebuilding the vibrational wavepacket in TRAS using attosecond X-ray pulses
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In situ characterization of few-cycle laser pulses in transient absorption spectroscopy
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Self-citationPotential Energy Surfaces of Core-Hole and Shake-Up States for Dissociative Ionization Studies
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Self-citationImpact of intense laser pulses on the autoionization dynamics of the 2s2p doubly excited state of He
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Perturbed ac Stark Effect for Attosecond Optical-Waveform Sampling
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Self-citation
- 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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