As expected, coverage increases as the population size increases. Having a larger population size allows for more traits in the generation to select from during crossover and allows for efficient exploration. Examining the coverage among each run (ESI Table ) indicates that the GA has difficulty finding high performers when optimizing the optical bandgap, most likely due to the more diverse search space. Increasing the population size to 72 or 96 allowed the GA to find 99-100% of the top 100 candidates for polarizability.