Molecules of the title compounds, 3'-methylacetanilide [or N-(m-tolyl)acetamide], C(9)H(11)NO, (I), and N-benzylthioacetamide, C(9)H(11)NS, (II), are connected by a framework of intermolecular N-H...O and N-H...S hydrogen bonds, respectively, forming chains with the graph-set description C(4), which run along the b axis. Analyses of the crystal structures of (I) and (II) are helpful in the elucidation of a generation mechanism of the IR spectra of hydrogen-bonded molecular crystals. The correlation between the IR spectra of studied compounds and structural data is also discussed.
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