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The mol­ecules of 2-amino-4,6-bis­[N-methyl-N-(4-methyl­phenyl)amino]pyrimidine-5-carbaldehyde, C21H23N5O, (I), and 2-amino-4-(indolin-1-yl)-6-methoxy­pyrimidine-5-carbaldehyde, C14H14N4O2, (II), which crystallizes with Z' = 2 in the space group P\overline{1}, exhibit polarized electronic structures. Mol­ecules of (I) are linked by a combination of N-H...O, C-H...O and C-H...[pi](arene) hydrogen bonds into a three-dimensional framework structure, while those of (II) are linked into sheets by a combination of two N-H...O hydrogen bonds and one N-H...[pi](arene) hydrogen bond.
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