The dataset includes all trajectories of the nonadiabatic molecular dynamics simulations of pyrene. Each tar.gz directory contains two directories: INPUT and RESULTS. In the INPUT directory, one has the input files for the Newton-X dynamics calculations and the subdirectory JOB_AD with the inputs for the ADC(2) calculations with TURBOMOLE. One also has the files "final_output.1.2" and "final_output.1.3" with the data used to obtain the emission spectrum. In the RESULTS directory, one has the 20 trajectories for the S2 state and 52 trajectories initiated in S7-S8. For the latter, the trajectories numbered 1-32 started in S7, and those numbered 33-52 started in S8. One also has a directory called TRAJ1_uncorrected that corresponds to the data for TRAJ1 without the kinetic energy correction. The RESULTS directory contains all the output files from the Newton-X dynamics calculation, including the file dyn.out with the atomic coordinates, velocities, and energies for each time step. There is also a file called "get_points.py," a python script used to extract the data (from the dyn.out files) for the emission spectrum.

Acknowledgments: S.M and M.B. thank the European Research Council (ERC) advanced grant SubNano (Grant agreement 832237) and the Centre de Calcul Intensif d'Aix-Marseille. E.V. thanks the Brazilian agencies CAPES for funding the grant through the Capes/PrInt project (Grant number 88887.467063/2019-00). E.V. and S. A. M. thank the Brazilian agency CNPq (Grant Numbers 423112/2018-0, 308371/2021-6 and 310123/2020-8) for support. I. B. thanks the Brazilian agencies CNPq (Grant numbers 304148/2018-0 and 409447/2018-8) and Faperj (Grant number E26/201.197/2021) for support.