Cited by 1,312Laser-Matter Interactions and ApplicationsAtomic and Molecular PhysicsSpectroscopy and Quantum Chemical Studies

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Real-time observation of valence electron motion

Goulielmakis, Eleftherios, Loh, Zhi-Heng, Wirth, Adrian, Santra, Robin, Rohringer, Nina, Yakovlev, Vladislav S., Zherebtsov, Sergey, Pfeifer, Thomas, Azzeer, Abdallah M., Kling, Matthias F., Leone, Stephen R., Krausz, Ferenc·2010·Nature

DOI 10.1038/nature09212

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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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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: Goulielmakis, Eleftherios
Loh, Zhi-Heng
Santra, Robin
Rohringer, Nina
Yakovlev, Vladislav S.
Zherebtsov, Sergey
Pfeifer, Thomas
Azzeer, Abdallah M.
Kling, Matthias F.
Leone, Stephen R.
Krausz, Ferenc
Venue: Nature
Publisher: Springer Science and Business Media LLC
Published: 2010-08
Volume: 466
Issue: 7307
Pages: 739-743
ISSN: 0028-0836 (ISSN-L)
1476-4687
DOI: 10.1038/nature09212
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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