We report the observation of extensive a- and c-type rotation-tunneling (RT
) spectra of (D2O)(2) for K-a = 0-4. These data allow quantification of mol
ecular constants and tunneling splittings for a number of previously unobse
rved RT states of (D2O)(2). The vibrational ground state has thus been char
acterized to energies as high as those of some of the intermolecular vibrat
ions, and we present the first test of the VRT(ASP-W) potential at these hi
gh K-a states.