Abstract: | In 5-benzyl-1,7-dimethyl-4,5,6,7-tetrahydro-1H-pyrazolo[3,4-d]pyrimidine-4,6-dione, C14H14N4O2, which crystallizes in space group P, weak intermolecular C—H⋯O hydrogen bonds generate dimers. The isomeric compound 1-benzyl-5,7-dimethyl-4,5,6,7-tetrahydro-1H-pyrazolo[3,4-d]pyrimidine-4,6-dione, C14H14N4O2, crystallizes in space group P21/n, and shows no such dimerization. Instead, it exhibits C—H⋯π interactions with the phenyl ring. In both structures, the molecules are linked by aromatic π–π-stacking interactions. |