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DOE OSTI · 1869495

Sensing ultrashort electronic coherent beating at conical intersections by single-electron pulses

Asban, Shahaf·Keefer, Daniel·Chernyak, Vladimir Y.·Mukamel, Shaul
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Abstract

In a theoretical study, we present an ultrafast technique for probing time-dependent molecular charge densities. An ultrafast optical pump first brings the molecule into an electronic nonstationary state. This is followed by coherent inelastic scattering of a broadband single-electron probe pulse with a variable delay T, which is detected spectrally. The technique is applied to reveal phase-sensitive background-free coherent electron beating in the conical intersection passage in uracil and reveals the otherwise elusive coherent beating of strongly coupled electrons and nuclei.

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71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICSconical intersectionssingle-electron spectroscopyultrafast dynamics

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Asban, Shahaf, Keefer, Daniel, Chernyak, Vladimir Y., Mukamel, Shaul. 2022-05-24. Sensing ultrashort electronic coherent beating at conical intersections by single-electron pulses. https://doi.org/10.1073/pnas.2205510119

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