Attosecond spectroscopy of molecular charge transfer uncovers a 1.5-fs delay in population transfer

Danylo T. Matselyukh, Florian Rott, Thomas Schnappinger (), Pengju Zhang, Zheng Li, Jeremy O. Richardson, Regina Vivie-Riedle and Hans Jakob Wörner ()
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Danylo T. Matselyukh: ETH Zürich
Florian Rott: LMU Munich
Thomas Schnappinger: LMU Munich
Pengju Zhang: ETH Zürich
Zheng Li: Peking University
Jeremy O. Richardson: ETH Zürich
Regina Vivie-Riedle: LMU Munich
Hans Jakob Wörner: ETH Zürich

Nature Communications, 2025, vol. 16, issue 1, 1-8

Abstract: Abstract The transfer of population between two intersecting quantum states is the most fundamental event in many dynamical processes in physics, chemistry, biology, and material science. Any two-state description of such processes requires population leaving one state to instantaneously appear in the other. We show that coupling to additional states, present in all real-world systems, can cause a measurable delay in population transfer. Using attosecond spectroscopy supported by quantum-chemical calculations, we measure a delay of 1.46 ± 0.41 fs at a charge-transfer crossing in CF3I+, where an electron hole moves from the fluorine atoms to iodine. Our measurements also resolve the other fundamental quantum-dynamical processes involved in the charge-transfer reaction: a vibrational rearrangement time of 9.38 ± 0.21 fs (during which the vibrational wave packet travels to the state crossing) and a population-transfer time of 2.3–2.4 fs. Our work shows that delays in population transfer readily appear in otherwise-adiabatic reactions and predicts them to be on the order of a single-femtosecond for molecular valence-state crossings. These results have implications for many research areas, such as atomic and molecular physics, charge transfer, or light harvesting.

Date: 2025
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DOI: 10.1038/s41467-025-62162-6

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