The largest cluster systems routinely studied using QC methods have been limited to roughly eight molecules. In cluster dynamics simulations, it is inferred that cluster sizes larger than eight molecules are stable against evaporation. However, it has not unambiguously been identified whether this is sufficient, and larger cluster systems are required to understand the cluster-to-particle transition regime. We recently pushed this limit by studying large (SA) n (AM) n clusters with up to 60 molecules (n = 30). We identified that more exhaustive sampling methodologies, compared to the usual state-of-the-art, might be required to accurately model such large clusters. Unfortunately, the computational cost increases exponentially with the growth of system size. Unlike crystals or 2D periodic materials, large clusters are not stable periodic systems. In addition, the high complexity of their configurational space is not only caused by the cluster size but also by various cluster compositions.