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Reaction of barbituric acid derivatives and di-substituted benzaldehyde in water afforded arylidene-1,3-dimethylpyrimidine-2,4,6(1H,3H,5H)-trione derivatives (1 and 2). The one step reaction proceeded efficiently, smoothly, and in excellent yield. The arylidene compounds were characterized by spectrophotometric tools plus X-ray single crystal diffraction technique. Quantum chemical calculations were performed using the DFT/B3LYP method to optimize the structure of the two isomers (1 and 2) in the gas phase. The optimized structures were found to agree well with the experimental X-ray structure data. The highest occupied (HOMO) and lowest unoccupied (LUMO) frontier molecular orbitals analyses were performed and the atomic charges were calculated using natural populationanalysis

Molecular Structure, Spectroscopic and DFT Computational Studies of Arylidene-1,3-dimethylpyrimidine-2,4,6(1H,3H,5H)-trione