[Electronic structure of helium and hydride complexes]

Research on the electronic structure of weakly bound helium and hydrogen species is described. The work grew from interest in a remarkable experimental observation at Los Alamos which shows that the helium generated from radioactive decay of liquid tritium remains in solution at concentrations which exceed the known solubility by much more than a factor of 100. The understanding of this supersolubility phenomenon is a challenging problem with significant implications for other condensed phase systems. In the hope of discovering the mechanism of the supersolubility, electronic structure calculations were carried out employing several methods to evaluate the binding energies of complexes of the form He(H+) (H2)/sub n/, with n = 2, 3, 4. For comparison, similar calculations were made for the complexes H2(H+) (H2)/sub n/. Also, the binding of the negative counter-ion species of the form (H-) (H2)/sub n/ was calculated. Although the calculations show that such complexes have sufficient binding energy to account for the enhanced solubility at the low temperature (20 K) of interest, major questions remain to be clarified. These include the mechanism for formation of the complexes, which may well involve excited, Rydberg-like states in solution. Another quite crucial question is how such weak complexes could persist in solution for months without displacement of the He by solvent molecules. Theoretical calculations focus on three topics: (1) Rydberg states; (2) condensed phase interactions; and (3) estimates of ionic conductivity in tritium solutions, as an aid to the interpretation of experiments now underway at Los Alamos