The first layer was decomposed into 3 clusters, followed by two for all remaining layers. Of course, the present choice of ML-trees is just a subset of in principle possible trees, picked by intuition and serving the purpose of comparison. Below we will discuss the performance and convergence of the different ML-trees in terms of the total (singlet + triplet) MLCT population. The connection to the overall dynamics is provided in Fig. . These results were obtained with tree (IV), which gave the best and) (V). The graphs are labeled according to the convergence threshold set p NO × 1000. The tightest convergence criteria for model (IV) of 0.2% will be set as a reference. Notice that in all curves there is a slight initial rise, which is discussed in ESI † Sec. S7. performance as will be detailed below. In Fig. one observes the expected behavior for this type of system. Initially, the laser pulse excited the 1 MLCT states which rapidly convert into MLCT states due to intersystem crossing. Internal conversion subsequently leads to a population relaxation in the triplet manifold towards the low-lying 3 MC states. Depopulation of MLCT states in the excitation window takes place within a few hundred femtoseconds, which is in accord with the experimental observation by Moll et al. In what follows, the convergence behaviour of the five ML-trees is investigated by gradually decreasing the threshold for p NO . In Fig. (a) the total MLCT population for tree (IV) is shown for p NO ranging from 5% to 0.2%. Only minor differences are observed between the two curves with the tightest convergence criteria. We therefore take the curve with the tightest convergence criteria as a reference to compare them against the remaining models.