Calculations at the MP2/6-31G* level for 2,7-diazatetracyclo[6.2.2.2(3,6)]tetradecane dication (1(2+)) give charges at each nitrogen of +0.06, at each CalphaH group of +0.23, and at each CbetaH2 group of +0.12. The increases in charge upon removal of two electrons from the neutral hydrazine are +0.86 at both nitrogens, +0.23 at all four CalphaH groups, and +0.91 at all eight CbetaH2 groups. The near-UV optical spectra of 1(2+) and 3(2+) show broad long-wavelength absorption near 300 nm (epsilon similar to 1700 M(-1) cm(-1) between similar to 295 and 320 nm for 1(2+) and 3(2+)) and stronger short-wavelength absorption (epsilon 5500 at 230 nm for 1(2+) and epsilon similar to 3100 at 222 nm for 3(2+)). Clark and Chandrasekar’s configuration interaction method using AM1 calculations predicts that the long-wavelength band should be assigned to a sigma --> pi* transition and that more intense sigma --> pi*, pi --> pi*, and sigma --> sigma* transitions all might contribute to the shorter-wavelength band, Comparisons of CIS/6-31G* and CC-CI/AM1 calculations on tetramethylhydrazine dication show good agreement of orbital ordering and oscillator strengths, brit very poor agreement of transition energies (pi --> pi* calculated at 151 and 265 nm, respectively).