Stereoselective Synthesis, Structural and Spectroscopic Study of 4,5,11-Triazatricyclo[6.2.1.02,6]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 P1¯. The structure is further stabilized by an intermolecular CH…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, 1H‐NMR and 13C‐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.