Experimental data of pentacene single crystals: Femtosecond electron diffraction data of pentacene single crystals measured at the Fritz Haber Institute in Berlin.The dataset contains an experiment for a long time range (measurement_1) and another experiment for a short time range (measurement_2). Theory data of pentacene single crystals: DFT - relaxation data obtained with Octopus and FHI-AIMS codes. Initial settings and resulting structures are included. This folder also contains results of phonons calculations performed with FHI-AIMS and Phonopy. md - this folder contains MD settings as well as obtained trajectories of equilibrium and out of equilibrium calculations. In each case, results of six parallel runs are included. diffraction - the folder contains diffraction data obtained from each of the six parallel runs, where the molecular dynamics trajectories were sampled every 250 fs. Data are divided for “equilibrium” and “out_of_equilibrium” sub folders. The diffraction data is stored in "out.npz" files that requires Python and NumPy to access. TDDFT - contains TDDFT results obtained with Octopus code. The “td.general” contains laser pulse data and atomic trajectories during the simulation.

Acknowledgments: this work was funded by the Max Planck Society, the European Research Council (ERC) under the European Unions Horizon 2020 research and innovation program (Grant Agreement Number ERC-2015-CoG-682843), and by the Deutsche Forschungsgemeinschaft (DFG) - Projektnummer 182087777 - SFB 951 (B17 and A13). H.S. acknowledges support by the Swiss National Science Foundation under Grant No. P2SKP2184100. Y.W.W acknowledges funding from the DFG within the Emmy Noether program under Grant No. RE 3977/1. M.K. acknowledges funding from the BigMAX Max Planck research network on big-data-driven material science. S.H. and J.P. are grateful to the DFG for support within project PF385/12 as well as to the Bavarian State Ministry for Science and the Arts for funding within the collaborative research network "Solar Technologies go Hybrid" (SolTech).