The melting mechanism of the Co(hmba)3[CoBr4] system as well as that with 0, 1, 2, or 3 water molecules added was further studied by ab initio molecular dynamics simulations. We are restricted to studying the crystal/molten state as the quenching to a glassy state (with a fairly low cooling rate) is computationally infeasible. First, we considered dynamics of the pristine, waterfree crystal structure (as obtained from its CIF file) at temperatures of 500, 1000, and 1500 K to Co-O CN (-)