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Real-time observation of valence electron motion
Abstract
The superposition of quantum states drives motion on the atomic and subatomic scales, with the energy spacing of the states dictating the speed of the motion. In the case of electrons residing in the outer (valence) shells of atoms and molecules which are separated by electronvolt energies, this means that valence electron motion occurs on a subfemtosecond to few-femtosecond timescale (1 fs = 10(-15) s). In the absence of complete measurements, the motion can be characterized in terms of a complex quantity, the density matrix. Here we report an attosecond pump-probe measurement of the density matrix of valence electrons in atomic krypton ions. We generate the ions with a controlled few-cycle laser field and then probe them through the spectrally resolved absorption of an attosecond extreme-ultraviolet pulse, which allows us to observe in real time the subfemtosecond motion of valence electrons over a multifemtosecond time span. We are able to completely characterize the quantum mechanical electron motion and determine its degree of coherence in the specimen of the ensemble. Although the present study uses a simple, prototypical open system, attosecond transient absorption spectroscopy should be applicable to molecules and solid-state materials to reveal the elementary electron motions that control physical, chemical and biological properties and processes.
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“Transient-absorption measurements at synchrotrons and in laboratory table-top systems in the XUV and x-ray were developed first, and the method was only applied to attosecond transient absorption in 2010 [222].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [222]
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Metadata
- Authors
- Goulielmakis, E., Loh, Z.-H., Wirth, A., Santra, R., Rohringer, N., Yakovlev, V. S., Zherebtsov, S., Pfeifer, T., Azzeer, A. M., Kling, M. F., Leone, S. R., & Krausz, F.
- Affiliations
- Max Planck Society (DE)
- Lawrence Berkeley National Laboratory (US)
- Argonne National Laboratory (US)
- Lawrence Livermore National Laboratory (US)
- King Saud University (SA)
- Corresponding author
- Goulielmakis, Eleftherios
- Leone, Stephen R.
- Krausz, Ferenc
- ORCID
- Venue
- Nature
- Published
- 2010-08
- Volume
- 466
- Issue
- 7307
- Pages
- 739-743
- ISSN
- 0028-0836 (ISSN-L)
- 1476-4687
- OpenAlex
- W1984246545
- Cited by
- 1,312
- References
- 30
- Citations by year
- 2026: 64 · 2025: 78 · 2024: 78 · 2023: 62 · 2022: 70 · 2021: 80 · 2020: 92 · 2019: 71 · 2018: 79 · 2017: 79 · 2016: 109 · 2015: 80 · 2014: 101 · 2013: 111 · 2012: 86
- FWCI
- 46.05
- Type
- journal article
- Language
- en
- Open access
- closed
- Licence
- www.springer.com/tdm (tdm)
- Locations
- Nature (publishedVersion)
- PubMed (publishedVersion)
- RePEc: Research Papers in Economics (submittedVersion)
- Desy publication database (The Deutsches Elektronen-Synchrotron) (submittedVersion)
- Max Planck Institute for Plasma Physics (submittedVersion)
- The HKU Scholars Hub (University of Hong Kong) (submittedVersion)
- MPG.PuRe (Max Planck Society) (submittedVersion)
- 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 › Spectroscopy and Quantum Chemical Studies
- Keywords
- attosecond transient absorption spectroscopy, valence electron dynamics, electron wave packets, krypton ions, attosecond pump-probe, electron density matrix, electron coherence, extreme ultraviolet pulses
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