Statistics-Based Design of Multicomponent Molecular Crystals with the Three-Center Hydrogen Bond

A statistical survey was carried out to determine the probability for combinations of specific CO and NH groups to form a three-center hydrogen bond between one CO and two NH groups. The results show significantly higher probabilities for charged CO⁻ groups. These results were utilized to prepare six multicomponent crystals that exploit the three-center hydrogen bond mainly through the R₄²(8) motif.