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arXiv · 2209.04330

Non-Adiabatic Electronic and Vibrational Ring-Opening Dynamics resolved with Attosecond Core-Level Spectroscopy

S. Severino·K. M. Ziems·M. Reduzzi·A. Summers·H. -W. Sun·Y. -H. Chien·S. Gräfe·J. Biegert
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Abstract

Non-adiabatic dynamics and conical intersections play a central role in the chemistry of most polyatomic molecules, ranging from isomerization to heterocyclic ring opening and avoided photo-damage of DNA. Studying the underpinning correlated dynamics of electronic and nuclear wave packets is a major challenge in real-time and, many times involves optically dark transient states. We show that attosecond core-level spectroscopy reveals the pathway dynamics of neutral furan across its conical intersections and dark states. Our method measures electronic-nuclear correlations to detect the dephasing of electronic coherence due to nuclear motion and identifies the ring-opened isomer as the dominant product. These results demonstrate the efficacy of attosecond core level spectroscopy as a potent method to investigate the real-time dynamics of photochemical reaction pathways in complex molecular systems.

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S. Severino, K. M. Ziems, M. Reduzzi, A. Summers, H. -W. Sun, Y. -H. Chien, S. Gräfe, J. Biegert. 2022-09-09. Non-Adiabatic Electronic and Vibrational Ring-Opening Dynamics resolved with Attosecond Core-Level Spectroscopy. https://doi.org/10.1038/s41566-024-01436-9

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