The workflow of the GA is seen in Figure . The dataset used as a starting point for GA runs consists of 91 ligands obtained from Meyer et al. including phosphines, pyridines and carbenes. From this dataset a pre-screening is performed followed by the score evaluation of catalyst structures which is used to determine the most promising ligands. The crossover and mutation operations follows the scheme presented by Jensen . Catalysts resulting from crossover are restricted to have between 2 and 100 heavy atoms and a maximum of 20 rotatable bonds. For a crossover operation between two catalysts (Figure Crossover), one of the two catalysts is selected as the catalyst to be modified (Cat 1 in Figure ). Then, a ligand is at random selected from this catalyst and combined with the corresponding ligand type in the other catalyst. Each new catalyst after crossover will in this way have modified either the anionic or the neutral ligand, while keeping the other ligand unchanged. This prevents the crossover procedure from being too disruptive on the catalysts and enables steady evolution. For further details on the crossover operations see Figure in section S4 in the SI. ligand dataset and passed to the algorithm. A detailed description of the crossover operations can be found in the SI.