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Computer simulation has long been an essential partner of ultrafastexperiments, allowing the assignment of microscopic mechanistic detail tolow-dimensional spectroscopic data. However, the ability of theory to make apriori predictions of ultrafast experimental results is relatively untested.Herein, as a part of a community challenge, we attempt to predict the signal ofan upcoming ultrafast photochemical experiment using state-of-the-art theory inthe context of preexisting experimental data. Specifically, we employ ab initioEhrenfest with collapse to a block (TAB) mixed quantum-classic simulations todescribe the real-time evolution of the electrons and nuclei of cyclobutanonefollowing excitation to the 3s Rydberg state. The gas-phase ultrafast electrondiffraction (GUED) signal is simulated for direct comparison to an upcomingexperiment at the Stanford Linear Accelerator Laboratory. Following initialring-opening, dissociation via two distinct channels is observed: the C3dissociation channel, producing cyclopropane and CO, and the C2 channel,producing CH$_2$CO and C$_2$H$_4$. Direct calculations of the GUED signalindicate how the ring-opened intermediate, the C2 products, and the C3 productscan be discriminated in the GUED signal. We also report an a priori analysis ofanticipated errors in our predictions: without knowledge of the experimentalresult, which features of the spectrum do we feel confident we have predictedcorrectly, and which might we have wrong?

Prediction challenge: First principles simulation of the ultrafast electron diffraction spectrum of cyclobutanone