Stereoselective Synthesis , Structural and Spectroscopic Study of 4,5,11‐Triazatricyclo[6.2.1.0*2,6*]Undec‐5‐ene

3‐(2,4‐Dichlorophenyl)‐7‐[(2,4‐dichlorophenyl)methylidene]‐11‐methyl‐4‐phenyl‐4,5,11‐triazatricyclo[6.2.1.0*2,6*]undec‐5‐ene ( 3 ) was synthesized in a stereoselective manner. Single crystal X‐ray study of 3 revealed that the structure belongs to the triclinic system with space group P 1 ¯ . The structure is further stabilized by an intermolecular CH … π interaction. Molecular mechanics force field (MM + ), followed by either semi‐empirical AM1 or PM3, was used to calculate the optimized geometrical parameters of 3 . The determined theoretical geometry parameters were found to be in good agreement with the parameters obtained by a single‐crystal study. Vibrational frequencies and gauge‐independent atomic orbital, 1 H‐NMR and 13 C‐NMR chemical shifts were computed at B3LYP/6‐31G(d) level of theory. Moreover, the molecular electrostatic potential of 3 has been calculated exhibiting that the most electrophilic site of 3 is the N‐3 atom; however, the nucleophilic site is distributed on the H atoms of dichlorophenyl groups. The frontier molecular orbitals of 3 have been determined by the same technique.