The starting atomic positions and velocities were taken from the ground state MD. All the details concerning the preparation of the non-adiabatic simulations can be found in the SI. and using the PBE0 functional as high level and the PBE functional as low level. In total 400 trajectories were thus obtained. Each simulation is stopped when a transition to the ground state occurs or when it reaches a region of the PES where the calculation fails to converge. Most simulations reach the ground state in less than 100 fs. The calculations that failed to converge have not been considered in the statistical analysis below. In the reference calculations, 7 failed to converge, while for the MTS runs 15, 5, and 9 failed to converge for the MTS factor 4, 6, and 8, respectively. This seems to indicate that the MTS algorithm does not affect the convergence of the calculations significantly.