Predictive theoretical photochemistry for X-ray probing of chemical bond dynamics

Recent advancements in laser technology and imaging techniques like X-ray free-electron lasers (XFELs) and ultrafast electron diffraction (UED) have revolutionized the study of ultrafast dynamics, enabling the probing of molecular structural changes with sub-Angstrom spatial and few-fs temporal resolution. Despite these advances, directly imaging the motion of individual atoms in photoinduced reactions remains challenging and often requires high-level theoretical calculations. Accurate computational simulations are essential not only for interpreting experimental results but also for the rational design of new experiments performed at XFEL facilities.

In our recent study, we highlight the crucial role of computational simulations in predicting experimental outcomes, particularly in the context of MeV-ultrafast electron diffraction techniques. We studied the ring-opening dynamics and photoproduct formation of photoexcited cyclobutanone, linking specific diffraction features to distinct photoproducts and their underlying structural dynamics. This approach provides valuable insights into the mechanisms governing various dissociation pathways, advancing our understanding of ultrafast photochemical processes.