ArticleProceedings of the National Academy of Sciences of the United States of America2021
Unveiling the spatial distribution of molecular coherences at conical intersections by covariance X-ray diffraction signals.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2021. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 6 papers.
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Who cites it
6 citing papers in PubMed.
- Simulation of time-resolved site-selective X-ray spectroscopy tracing nonadiabatic dynamics inPhysical chemistry chemical physics : PCCP · 2025Article
- Monitoring vibronic coherences and molecular aromaticity in photoexcited cyclooctatetraene with an X-ray probe: a simulation study.Chemical science · 2023Article
- Time-resolved X-ray and XUV based spectroscopic methods for nonadiabatic processes in photochemistry.Chemical communications (Cambridge, England) · 2022Review
- Probing nonadiabatic dynamics with attosecond pulse trains and soft x-ray Raman spectroscopy.Structural dynamics (Melville, N.Y.) · 2022Article
- Electronic coherences in nonadiabatic molecular photophysics revealed by time-resolved photoelectron spectroscopy.Proceedings of the National Academy of Sciences of the United States of America · 2022Article
- Transient measurement of phononic states with covariance-based stochastic spectroscopy.Light, science & applications · 2022Article
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7 authors.
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Abstract
The outcomes and timescales of molecular nonadiabatic dynamics are decisively impacted by the quantum coherences generated at localized molecular regions. In time-resolved X-ray diffraction imaging, these coherences create distinct signatures via inelastic photon scattering, but they are buried under much stronger background elastic features. Here, we exploit the rich dynamical information encoded in the inelastic patterns, which we reveal by frequency-dispersed covariance ultrafast powder X-ray diffraction of stochastic X-ray free-electron laser pulses. This is demonstrated for the photoisomerization of azobenzene involving the passage through a conical intersection, where the nuclear wave packet branches and explores different quantum pathways. Snapshots of the coherence dynamics are obtained at high frequency shifts, not accessible with conventional diffraction measurements. These provide access to the timing and to the confined spatial distribution of the valence electrons directly involved in the conical intersection passage. This study can be extended to full three-dimensional imaging of conical intersections with ultrafast X-ray and electron diffraction.
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