We have argued that the space of unexplored PSs is vast, with considerable potential for finding high-quality semiconductors. Computational screening methods based on high-throughput DFT are a useful tool to search for materials with the desired properties in large chemical spaces. However, some of the key properties that are linked to high PV performance (most notably τ) are prohibitively expensive to calculate for more than a handful of materials. Additionally, many physical effects that are likely to affect the experimental τ (defect clusters, entropic effects, grain boundaries etc.) have to be neglected to make the problem computationally treatable. Finally, it is challenging to predict the properties of hypothetical materials with unknown crystal structures, because both composition and structure are required in first-principles calculations as input. Many hypothetical PSs with P/S > 1 and many hypothetical quaternary PSs have unknown crystal structures. Thus, we argue that high-throughput experiments are necessary to rapidly explore the synthesizability and properties of known and unknown PS semiconductors.