X-ray imaging of chemically active valence electrons during a pericyclic reaction

Abstract

Time-resolved imaging of chemically active valence electron densities is a long sought goal, as these electrons dictate the course of chemical reactions. However, x-ray scattering is always dominated by the core and inert valence electrons, making time-resolved x-ray imaging of chemically active valence electron densities extremely challenging. To image such electron densities, we demonstrate an effective and robust method, which emphasizes the information encoded in weakly scattered photons. The degenerate Cope rearrangement of semibullvalene, a pericyclic reaction, is used as an example to visually illustrate our approach. Our work also provides experimental access to the long-standing problem of synchronous versus asynchronous bond formation and breaking during pericyclic reactions.

arXiv comment19 pages, 3 figures, comments are most welcome

References in corpus (6)

• X-ray diffraction from isolated and strongly aligned gas-phase molecules with a free-electron laser
• Imaging electronic quantum motion with light
• Time-dependent electron localization function
• Laser-induced 3D alignment and orientation of quantum-state-selected molecules
• Theory of time-resolved non-resonant x-ray scattering for imaging ultrafast coherent electron motion
• Role of electron-electron interference in ultrafast time-resolved imaging of electronic wavepackets

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