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

Shahaf Asban; Daniel Keefer; Vladimir Y Chernyak; Shaul Mukamel

doi:10.1073/pnas.2205510119

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

Proc Natl Acad Sci U S A. 2022 May 31;119(22):e2205510119. doi: 10.1073/pnas.2205510119. Epub 2022 May 24.

Authors

Shahaf Asban^{1

2}, Daniel Keefer^{1

2}, Vladimir Y Chernyak^{3

4}, Shaul Mukamel^{1

2}

Affiliations

¹ Department of Chemistry, University of California, Irvine, CA 92697-2025.
² Department of Physics & Astronomy, University of California, Irvine, CA 92697-2025.
³ Department of Chemistry, Wayne State University, Detroit, MI 48202.
⁴ Department of Mathematics, Wayne State University, Detroit, MI 48202.

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 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.

Keywords: conical intersections; single-electron spectroscopy; ultrafast dynamics.

Publication types

Research Support, Non-U.S. Gov't
Research Support, U.S. Gov't, Non-P.H.S.