The required convergence threshold and the speed at which convergence is achieved depend strongly on the structure of the ML-tree. This can be seen by comparing the different panels of Fig. . In all cases, the not sufficiently converged results show a slower decay of the MLCT population, i.e. in particular a trapping of population in high-lying excited triplet states. Increasing the convergence threshold will lead the dynamics trending towards the reference results, although with varying speeds (to make that this is not a feature of the particular model, it has been checked for a 42-dimensional model, see ESI † Fig. ).