The electronic and optical properties of most of the materials in the PAH101 set have not been thoroughly investigated experimentally. Some of the quantities calculated here, such as triplet excitation energies, are difficult to probe experimentally and require highly specialized techniques and facilities. Therefore, although the PAH101 set is relatively small, it is possible that some useful materials would be found in it. Here, we provide examples for some of the electronic and optical properties relevant for organic electronic devices that can be extracted from the dataset. The dataset can be searched for materials with a particular property or combination of properties. As demonstrated below, the dataset may provide insights on structure-property relations and expose gaps in our understanding of the properties of molecular crystals that call for further investigation. One of the key properties for device applications is the optical gap, whose distribution in the dataset is shown in Figure .