The PAH101 set contains materials with a wide range of optical gaps. Crystalline quaterrylene (QUATER10) and hexacene (ZZZDKE01) have the smallest optical gaps of 1.33 eV and 1.17 eV, respectively. If a material is sought with an optical gap of up to about 5 eV it may be found in the dataset. Absorption spectra for light polarized along the three crystal axes are also provided in the dataset (see Table ), such that materials can be sought with broad absorption and/or absorption peaks in certain energy ranges.