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Tracing Long-Lived Atomic Coherences Generated via Molecular Conical Intersections

Patrick Rupprecht1,2,*,†, Francesco Montorsi3,*,‡, Lei Xu4, Nicolette G. Puskar1,2, Marco Garavelli3, Shaul Mukamel5, Niranjan Govind4,6, Daniel M. Neumark1,2,§, Daniel Keefer7,∥ et al.

Stephen R. Leone1,2,8,¶

  • *These authors contributed equally to this work.
  • †Contact author: prupprecht@lbl.gov
  • ‡Contact author: francesco.montorsi4@unibo.it
  • §Contact author: dneumark@berkeley.edu
  • ∥Contact author: keeferd@mpip-mainz.mpg.de
  • Contact author: srl@berkeley.edu
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Phys. Rev. Lett. 135, 233201 – Published 5 December, 2025

DOI: https://doi.org/10.1103/6bfk-mgpn

Abstract

Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections, which generate coherences between electronic states in molecules. We show with accurate calculations performed on gas-phase methyl iodide that electronic coherences of spin-orbit-split states persist in atomic iodine after dissociation. Our simulation predicts a maximum magnitude of vibronic coherence in the molecular regime of 0.75% of the initially photoexcited state population. Upon dissociation, one-third of this coherence magnitude is transferred to a long-lived atomic coherence where vibrational decoherence can no longer occur. To trace these dynamics, we propose a tabletop experimental approach—heterodyned attosecond four-wave-mixing spectroscopy. This technique can temporally resolve small electronic coherence magnitudes and reconstruct the full complex coherence function via phase cycling. Hence, heterodyned attosecond four-wave-mixing spectroscopy leads the way to a complete understanding and optimal control of spin-orbit-coupled electronic states in photochemistry.

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Phys. Rev. Lett. 135, 233201– Published 5 December, 2025
  • Received 8 April 2025
  • Accepted 16 October 2025
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