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

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.

References in corpus (5)

• Imaging the Photochemical Ring-Opening of 1,3-Cyclohexadiene by Ultrafast Electron Diffraction
• Ultrafast X-ray spectroscopy of conical intersections
• Femtosecond Symmetry Breaking and Coherent Relaxation of Methane Cations at the Carbon K-Edge
• Probing the energy conversion pathways between light, carriers and lattice in real time with attosecond core-level spectroscopy
• Theoretical analysis of the role of complex transition dipole phase in XUV transient-absorption probing of charge migration

Cited by in corpus (1)

• Probing coherent electronic superpositions of singly- and doubly-excited states of krypton with attosecond four-wave mixing spectroscopy