Dataset for: Identifying Aspirin Polymorphs from Combined DFT-Based Crystal Structure Prediction and Solid-State NMR

A combined experimental and computational approach was used to distinguish between different polymorphs of the pharmaceutical drug aspirin. This method involves the use of Ab Initio Random Structure Searching (AIRSS), a DFT-based crystal structure prediction method for the high-accuracy prediction of polymorphic structures, with DFT calculations of NMR parameters and solid-state NMR experiments at natural abundance. AIRSS was used to predict the crystal structures of form-I and form-II of aspirin. The root-mean-square deviation (RMSD) between experimental and calculated 1H chemical shifts was used to identify form-I as the polymorph present in the experimental sample, the selection being successful despite the large similarities between the molecular environments in the crystals of the two polymorphs.