Attosecond core-level absorption spectroscopy reveals the electronic and nuclear dynamics of molecular ring opening

Severino, S., Ziems, K. M., Reduzzi, M., Summers, A., Sun, H. W., Chien, Y. H., Gräfe, S. and Biegert, J. (2024) Attosecond core-level absorption spectroscopy reveals the electronic and nuclear dynamics of molecular ring opening. Nature Photonics, 18 (7), 731-737. (doi:10.1038/s41566-024-01436-9).

Abstract

We show that attosecond core-level spectroscopy is a powerful tool for investigating molecular dynamics due to its combined attosecond temporal resolution and the broad coherent spectrum that allows deciphering the signatures of nuclear and electronic motion through their different energetic signatures. The method reveals that the correlated real-time electronic and nuclear wavepacket dynamics and non-adiabatic transitions across conical intersections identify electronic and nuclear coherences and directly register symmetry changes in the X-ray absorption spectrum. We demonstrate the method’s efficacy to unveil the entire time history of the ring-opening dynamics of furan. The investigation establishes attosecond core-level spectroscopy as a potent method to investigate the real-time dynamics of photochemical reaction pathways in molecular systems.

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Contributors

Author: K. M. Ziems

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