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

Asban, Shahaf; Keefer, Daniel; Chernyak, Vladimir Y; Mukamel, Shaul · Proc Natl Acad Sci U S A · 2022

basic_science · Level V

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Abstract

SignificanceIn 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 <i>T</i>, 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.