Then, the experiments using these ligands as well as PPh3 were performed, and the observed yields and selectivities were summarized in the table (Figure ). To our surprise, PPh3 exhibit higher α selectivity than DPEPhos, which was determined as the optimal ligand for α-selective hydrogermylation of 9a (Figure ). The observed selectivities were plotted against predicted values (Figure ), and a modertate correlation for all ligands were confirmed (R 2 = 0.59). Overall, the highest observed α selectivity was 73% for L2, and this value this value did not change when the catalyst loading was reduced to 1.5 mol%. Notably, L2 is less commercially available compared to other typical triarylphosphines probably because it is rapidly oxidized when the solution is exposed to air. Hence, it is unlikely to be included as an initial candidate for random screening of ligands. The VLAO method rapidly suggested important features of ligand, enabling us to find such an elusive ligand with a minimum number of experimental trials.