Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites

The detailed understanding of electronic coherence in quantum systems requires measurements on the attosecond timescale. Attosecond x-ray pulses enable the study of electronic coherence in core-excited molecular systems. Here we report on the coherent motion of electrons in the 1,1-difluoroethylene ion following ionization of the <a:math xmlns:a="http://www.w3.org/1998/Math/MathML" display="inline"><a:mi>K</a:mi></a:math> shell of the two nonequivalent carbon sites with a subfemtosecond x-ray pulse. Using the angular streaking technique to track the Auger-Meitner decay, we observe temporal modulations of the emission, indicating the electronic coherence of the core-excited ionic states, and extract a <c:math xmlns:c="http://www.w3.org/1998/Math/MathML" display="inline"><c:mn>6.5</c:mn><c:mo>±</c:mo><c:mn>0.8</c:mn><c:mtext> </c:mtext><c:mtext> </c:mtext><c:mi>fs</c:mi></c:math> average lifetime of the core-level vacancies. A quantum-mechanical model is employed to interpret the measurement, and we find the observed temporal modulations are independent of charge density oscillations. This work opens a new regime of coherent electronic motion, beyond charge migration, where electronic coherence manifests in the nonlocal quantum correlation between atomic sites while charge density oscillation is absent. Our results broaden the landscape of electronic coherence in molecular systems.

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Publication Details

Journal
Physical Review X
Published
2025-01-16
DOI
https://doi.org/10.1103/physrevx.15.011008
Citations
3
Primary Topic
Laser-Matter Interactions and Applications
Type
article
Field-Weighted Citation Impact
3.74

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article

Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites

Taran Driver, Sandra Beauvarlet, Xinxin Cheng, Agostino Marinelli et al.
3 citations
Physical Review X
Laser-Matter Interactions and Applications
3.74
article

Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites

Taran Driver, Sandra Beauvarlet, Xinxin Cheng, Agostino Marinelli, Erik Isele, David Cesar, Matthias C. Hoffmann, Oliver Alexander, Joseph Duris, P. H. Bucksbaum, Peter Walter, River Robles, Siqi Li, Ming‐Fu Lin, Kirk A. Larsen, J. P. Marangos, Philipp Rosenberger, Přemysl Kolorenč, James Cryan, James M. Glownia, Paul Hockett, Razib Obaid, Thomas Wolf, Kurtis Borne, Matthias F. Kling, Paris Franz, Zhaoheng Guo, Martin Graßl, Emily Thierstein, Xiang Li, Jun Wang, Andrei Kamalov, Louis F. DiMauro
article en
3 citations

Abstract

The detailed understanding of electronic coherence in quantum systems requires measurements on the attosecond timescale. Attosecond x-ray pulses enable the study of electronic coherence in core-excited molecular systems. Here we report on the coherent motion of electrons in the 1,1-difluoroethylene ion following ionization of the <a:math xmlns:a="http://www.w3.org/1998/Math/MathML" display="inline"><a:mi>K</a:mi></a:math> shell of the two nonequivalent carbon sites with a subfemtosecond x-ray pulse. Using the angular streaking technique to track the Auger-Meitner decay, we observe temporal modulations of the emission, indicating the electronic coherence of the core-excited ionic states, and extract a <c:math xmlns:c="http://www.w3.org/1998/Math/MathML" display="inline"><c:mn>6.5</c:mn><c:mo>±</c:mo><c:mn>0.8</c:mn><c:mtext> </c:mtext><c:mtext> </c:mtext><c:mi>fs</c:mi></c:math> average lifetime of the core-level vacancies. A quantum-mechanical model is employed to interpret the measurement, and we find the observed temporal modulations are independent of charge density oscillations. This work opens a new regime of coherent electronic motion, beyond charge migration, where electronic coherence manifests in the nonlocal quantum correlation between atomic sites while charge density oscillation is absent. Our results broaden the landscape of electronic coherence in molecular systems.

Physical Review XVol. 15(1)
Kansas State University (US), Charles University (CZ), SLAC National Accelerator Laboratory (US), Max Planck Institute of Quantum Optics (DE), National Research Council Canada (CA), Imperial College London (GB), The Ohio State University (US), Ludwig-Maximilians-Universität München (DE), Stanford University (US)
U.S. Department of Energy, Grantová Agentura České Republiky, Office of Science, Basic Energy Sciences, Workforce Development for Teachers and Scientists, Chemical Sciences, Geosciences, and Biosciences Division, SLAC National Accelerator Laboratory
Openalex Percentile: Top 9%
Laser-Matter Interactions and Applications
3.74
DOIOpen Access PDFOpenAlex
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