Imaging electronic quantum motion with light
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Imaging the quantum motion of electrons not only in real-time, but also in real-space is essential to understand for example bond breaking and formation in molecules, and charge migration in peptides and biological systems. Time-resolved imaging interrogates the unfolding electronic motion in such systems. We find that scattering patterns, obtained by X-ray time-resolved imaging from an electronic wavepacket, encode spatial and temporal correlations that deviate substantially from the common notion of the instantaneous electronic density as the key quantity being probed. Surprisingly, the patterns provide an unusually visual manifestation of the quantum nature of light. This quantum nature becomes central only for non-stationary electronic states and has profound consequences for time-resolved imaging.
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It has been demonstrated that, even at low intensity, ultrafast x-ray scattering from electron wavepackets can hold surprises, which derive from the impossibility to separate electronically elastic and inelastic scattering events when using ultrafast x-ray pulses [116].
“It has been demonstrated that, even at low intensity, ultrafast x-ray scattering from electron wavepackets can hold surprises, which derive from the impossibility to separate electronically elastic and inelastic scattering events when using ultrafast x-ray pulses [116].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [116]
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Cavaletto, S. M., Keefer, D., Rouxel, J. R., Aleotti, F., Segatta, F., Garavelli, M., & Mukamel, S. (2021) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.2105046118 · Cited by 19 · see citing works
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Self-citationTheory of x-ray scattering from laser-driven electronic systems
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Self-citationTime-resolved pump-probe spectroscopy to follow valence electronic motion in molecules: Application
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Time-resolved X-ray scattering by electronic wave packets: analytic solutions to the hydrogen atom
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Perveaux, A., Lauvergnat, D., Gatti, F., Halász, G. J., Vibók, Á., & Lasorne, B. (2014) · The Journal of Physical Chemistry A · doi:10.1021/jp508218n · Cited by 16 · see citing works
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Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy
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Self-citationImaging Electron Dynamics with Ultrashort Light Pulses: A Theory Perspective
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Visualising many-body electron dynamics using one-body densities and orbitals
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Imaging instantaneous electron flow with ultrafast resonant x-ray scattering
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Self-citationImaging population transfer in atoms with ultrafast electron pulses
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Self-citationScattering of X-ray Ultrashort Pulses by Complex Polyatomic Structures
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Stimulated X-ray Raman Imaging of Conical Intersections
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Towards high-resolution X-ray scattering as a probe of electron correlation
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Scattering of Ultrashort X-ray Pulses by Various Nanosystems
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Ultrafast Molecular Frame Quantum Tomography
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Comment on “How to observe coherent electron dynamics directly”
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Self-citationToward the Generation of an Isolated TW-Attosecond X-ray Pulse in XFEL
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Towards novel probes for valence charges via X-ray optical wave mixing
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Multidimensional scattering of attosecond x-ray pulses detected by photon-coincidence
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The development of attosecond XFELs for understanding ultrafast electron motion
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Scattering of Ultrashort X-ray Pulses on Diamonds with NV Centers
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Real-space inversion and super-resolution of ultrafast scattering
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Attosecond x-ray scattering from a particle-hole wave packet
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Time-resolved X-ray Scattering of Excited State Structure and Dynamics
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Energy-resolved coherent diffraction from laser-driven electronic motion in atoms
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Probing Electronic Symmetry Reduction during Charge Migration via Time‐Resolved X‐Ray Diffraction
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Self-citationScattering of Attosecond Laser Pulses on a DNA Molecule during Its Nicking and Bending
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Time-resolved x-ray scattering from impulsively aligned or oriented molecules
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Berrah, N., Cryan, J. P., Robles, R., Driver, T., Marinelli, A., & Bucksbaum, P. H. (2025) · Advances in Optics and Photonics · doi:10.1364/aop.540527 · Cited by 7 · see citing works
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- Authors
- Dixit, G., Vendrell, O., & Santra, R.
- Affiliations
- Deutsches Elektronen-Synchrotron DESY (DE)
- Universität Hamburg (DE)
- Venue
- Proceedings of the National Academy of Sciences
- Publisher
- National Academy of Sciences
- Published
- 2012-07-02
- Volume
- 109
- Issue
- 29
- Pages
- 11636-11640
- ISSN
- 0027-8424 (ISSN-L)
- 1091-6490
- PMC
- PMC3406851
- OpenAlex
- W2533628335
- Cited by
- 177
- References
- 43
- Citations by year
- 2026: 7 · 2025: 8 · 2024: 18 · 2023: 19 · 2022: 14 · 2021: 14 · 2020: 13 · 2019: 11 · 2018: 13 · 2017: 11 · 2016: 6 · 2015: 8 · 2014: 19 · 2013: 12 · 2012: 4
- FWCI
- 7.11
- Type
- journal article
- Language
- en
- Open access
- green
- www.ncbi.nlm.nih.gov
- Locations
- Proceedings of the National Academy of Sciences (publishedVersion)
- Europe PMC (PubMed Central) (publishedVersion)
- PubMed Central (publishedVersion)
- PubMed (publishedVersion)
- Desy publication database (The Deutsches Elektronen-Synchrotron) (publishedVersion)
- arXiv (Cornell University) (submittedVersion)
- arXiv (Cornell University)
- Topics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Physics and Astronomy › Radiation › Advanced X-ray Imaging Techniques
- Physical Sciences › Physics and Astronomy › Radiation › X-ray Spectroscopy and Fluorescence Analysis
- Keywords
- time-resolved X-ray imaging, electron wave packets, spatio-temporal correlation, quantum nature of light, bond breaking and formation, charge migration
- MeSH terms
- Electrons, Light, Models, Chemical, Quantum Theory, Radiography, Scattering, Radiation
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