The average-valence Cu-2(3+) Site in bis(copper) complexes with three azacryptands has been probed by electronic absorption, resonance Raman (RR), and magnetic circular dichroism (MCD) spectroscopy. The X-ray structure of one of the complexes is presented. RR excitation profiles of low-frequency Cu-Cu and Cu-N modes establish that at least two vibronic transitions contribute to the absorption intensity in the range 700-900 nm, in agreement with the MCD data and indicative of vibronic transitions involving substantial motion of both copper nuclei.