ArticleProceedings of the National Academy of Sciences of the United States of America2020
Visualizing conical intersection passages via vibronic coherence maps generated by stimulated ultrafast X-ray Raman signals.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2020. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 26 papers.
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26 citing papers in PubMed.
- Tutorial on Energy Transfer Mechanisms and Computational Methods in X‑ray Photodynamic Therapy with Metal Nanoclusters.ACS physical chemistry Au · 2026Article
- Capturing coherent pseudorotation through conical intersection in photoionized benzene.Nature communications · 2025Article
- Simulation of time-resolved site-selective X-ray spectroscopy tracing nonadiabatic dynamics inPhysical chemistry chemical physics : PCCP · 2025Article
- Unraveling the Relaxation Dynamics of Uracil: Insights from Time-Resolved X-ray Photoelectron Spectroscopy.Journal of the American Chemical Society · 2025Article
- Simulating Electronic Coherences Induced by Conical Intersections Using MASH: Application to Attosecond X-ray Spectroscopy.The journal of physical chemistry letters · 2025Article
- Direct All-Atom Nonadiabatic Semiclassical Simulations for Electronic Absorption Spectroscopy of Organic Photovoltaic Non-Fullerene Acceptor in Solution.The journal of physical chemistry letters · 2025Article
- A numerically exact description of ultrafast vibrational decoherence in vibration-coupled electron transfer.Proceedings of the National Academy of Sciences of the United States of America · 2025Article
- Controlling Electronic Coherences and the Curvature Induced by the Derivative Coupling at a Conical Intersection: A Quantum Ehrenfest (QuEh) Protocol for Reaction Path Following Application to "Channel 3" Benzene Photochemistry.The journal of physical chemistry. A · 2024Article
- Time-Resolved X-ray Absorption Spectroscopy: An MCTDH Quantum Dynamics Protocol.Journal of chemical theory and computation · 2024Article
- Nonlinear Molecular Electronic Spectroscopy via MCTDH Quantum Dynamics: From Exact to Approximate Expressions.Journal of chemical theory and computation · 2023Article
- 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
- Charge-induced chemical dynamics in glycine probed with time-resolved Auger electron spectroscopy.Structural dynamics (Melville, N.Y.) · 2022Article
- Decoherence and Revival in Attosecond Charge Migration Driven by Non-adiabatic Dynamics.Nature physics · 2022Article
- Electronic quantum coherence in glycine molecules probed with ultrashort x-ray pulses in real time.Science advances · 2022Article
- Ultrafast coherent photoexcited dynamics in a trimeric dendrimer probed by X-ray stimulated-Raman signals.Chemical science · 2022Article
- Sensing ultrashort electronic coherent beating at conical intersections by single-electron pulses.Proceedings of the National Academy of Sciences of the United States of America · 2022Article
- 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
- Photoisomerization transition state manipulation by entangled two-photon absorption.Proceedings of the National Academy of Sciences of the United States of America · 2021Article
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Abstract
The rates and outcomes of virtually all photophysical and photochemical processes are determined by conical intersections. These are regions of degeneracy between electronic states on the nuclear landscape of molecules where electrons and nuclei evolve on comparable timescales and thus become strongly coupled, enabling radiationless relaxation channels upon optical excitation. Due to their ultrafast nature and vast complexity, monitoring conical intersections experimentally is an open challenge. We present a simulation study on the ultrafast photorelaxation of uracil, based on a quantum description of the nuclei. We demonstrate an additional window into conical intersections obtained by recording the transient wavepacket coherence during this passage with an X-ray free-electron laser pulse. Two major findings are reported. First, we find that the vibronic coherence at the conical intersection lives for several hundred femtoseconds and can be measured during this entire time. Second, the time-dependent energy-splitting landscape of the participating vibrational and electronic states is directly extracted from Wigner spectrograms of the signal. These offer a physical picture of the quantum conical intersection pathways through visualizing their transient vibronic coherence distributions. The path of a nuclear wavepacket in the vicinity of the conical intersection is directly mapped by the proposed experiment.
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