The experimental PXRD pattern of the resulting, activated material was compared to the simulated patterns of the full set of predicted crystal structures using constrained dynamic time-warping (see SI for details), which highlights a high similarity of the activated material to the predicted structures in the 0.8 g/cm 3 spike on the CSP energy-density map (Figure ). Visual comparison shows that all of the evacuated samples match the simulated PXRD pattern of the predicted polymorph, 1 (Figure ; SI, Figures ). These results show the potential for automated matching of materials from HT crystallization screens against databases of predicted structures, which could rapidly identify likely structures of new materials. We next studied the transformation and activation in more detail using the THF/n-butylbenzene solvate (TMA_2-33). After complete exchange of the crystallization solvent with n-pentane, which was determined using H NMR (SI, Figure ), we used thermogravimetric analysis (TGA) to determine the n-pentane solvent evaporation rate from the crystal pores at room temperature (SI, Figure ). Using single crystal XRD, we showed that the pentane-solvated TMA_2-33 structure undergoes a single-crystal-to-single-crystal transformation to a solvent free form, TMA (Table , see SI, Table and Figure ). The crystal packing of TMA molecules in TMA are in excellent agreement with the predicted low density packing in, 1, (Table , Figure ), not only in the hexagonal packing on TMA molecules, but also in the stacking of these sheets.