The field of transition metal clusters has proven to be fertile ground for study in recent years due to their interesting properties and reactivity. In this thesis, Velocity Map Imaging (VMI) has been used alongside spectroscopic techniques to study a range of diatomic metal-containing molecules which have relevance to cluster chemistry. The photodissociation of Ag-RG complexes (RG = Ar, Kr, Xe), as well as AgO, have been studied in the 29900-31700 cm⁻¹1 spectral region using VMI. The electronic states of the fragments produced have been assigned in each case and new values for the dissociation energies determined. These are presented as an update to the most recent experimental values for each molecule, about which doubts have been expressed. VMI has also been used to study the photodissociation dynamics of isotopically-selected 98MoO and 52CrO in multiple spectral regions. Assignments have been proposed for the processes generating the observed features, and values for the dissociation energies of these species determined which are consistent with literature values from other, older experimental techniques, or indirect measurements. Finally, a comparison has been made of different image reconstruction algorithms in order to determine which is best suited to analysing the data recorded in our group. The experimental data from the rest of this thesis have been reanalysed using various approaches, and it is demonstrated that recently-developed maximum entropy programs produce better results than the onion peeling algorithm previously used.