DFT calculations are consistent with the fragmentation of 32 to 2 equiv. 3 being disfavoured in the absence of a coordinating solvent (G°298K = +46.1 kcal mol -1 ; H° = +66.3 kcal mol -1 ). Deaggregation becomes more favourable in the presence of THF with conversion of 32 + 4 THF → 2 3-THF2 being only modestly endergonic (G°298K = +8.5 kcal mol -1 ; H° = -20.4 kcal mol -1 ). In the presence of an excess THF (solvent) the equilibrium is likely displaced to the products, allowing the isolation of 3-THF 2 . DOSY NMR studies suggest that the nuclearity of 32 and 3-THF2 observed in the solid-state is potentially retained in solution. In C6D6 at 298 K the diffusion coefficient of 32 was measured as 7.8 x 10 -10 m 2 s -1 while 3-THF2 in THF-d8 solution diffused at a substantial faster rate 1.1 x 10 -9 m 2 s -1 . The data correspond to estimated hydrodynamic radii of 9.3 Å for 32 and 7.2 Å for 3-THF2 consistent with 32 retaining its tetrametallic structure in solution.