1.5-Femtosecond Delay in Charge Transfer

• URL: http://arxiv.org/abs/2408.17402v1
• Date: Fri, 30 Aug 2024 16:40:45 GMT
• Title: 1.5-Femtosecond Delay in Charge Transfer
• Authors: Danylo T. Matselyukh, Florian Rott, Thomas Schnappinger, Pengju Zhang, Zheng Li, Jeremy O. Richardson, Regina de Vivie-Riedle, Hans Jakob Wörner,
• Abstract summary: Transfer of population between two intersecting quantum states is the most fundamental dynamical event. We show that coupling to additional states, present in all real-world systems, can cause a measurable delay in population transfer. Results have implications for many research areas, such as atomic and molecular physics, charge transfer or light harvesting.
• Score: 4.584198603153748
• License: http://creativecommons.org/licenses/by-nc-nd/4.0/
• Abstract: The transfer of population between two intersecting quantum states is the most fundamental dynamical event that governs a broad variety of processes in physics, chemistry, biology and material science. Whereas any two-state description implies that population leaving one state instantaneously appears in the other state, 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 advanced quantum-chemical calculations, we measure a delay of 1.46$\pm$0.41 fs at a charge-transfer state crossing in CF$_3$I$^+$, where an electron hole moves from the fluorine atoms to iodine. Our measurements also fully resolve the other fundamental quantum-dynamical processes involved in the charge-transfer reaction: a vibrational rearrangement time of 9.38$\pm$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 experimental results and theoretical simulations show that delays in population transfer readily appear in otherwise-adiabatic reactions and are typically on the order of 1 fs for intersecting molecular valence states. These results have implications for many research areas, such as atomic and molecular physics, charge transfer or light harvesting.

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