The molecular structure and spectral properties of N-methyl-N-(4-pyridyl)-nitramine (1) and 1, 4-dihydro-1-methyl-4-nitriminopyridine (3) were investigated by the X-ray diffraction, FTIR, nuclear magnetic resonance (NMR) methods and DFT theoretical calculations. N-methyl-N- (4-pyridyl)-nitramine (1) crystallises in the orthorhombic Pbca space group. It is composed of two planar fragments; nitramino (N2O2) group and the pirydyl ring. These two groups are ...