Crystal structure landscapes from combined vibrational spectroscopy and ab initio calculations: 4-(Dimethylamino)benzaldehyde

The method is successfully applied to the elucidation of 4-(dimethylamino)benzaldehyde crystal structure, considered to be “unknown” to illustrate the applicability of the PiMM approach. The proposed crystal structure, based on weak CH⋯O hydrogen bonding and π-stacking interactions, is in full agreement with the recently reported crystal structure.