This dissertation concerns the use of bicyclic guanidinate ligands to prepare new dimetal paddlewheel compounds. Specifically, Ru₂ ⁶⁺, Re₂⁶⁺, Re₂⁷⁺, and Os₂⁷⁺ compounds will be examined to observe any changes brought about by using bicyclic guanidinate ligands with varying ring sizes. In the Ru₂⁶⁺ compounds, different ligand ring sizes cause a change in the electronic configuration and magnetic properties. Bicyclic guanidinate ligands allow the preparation of Re₂ ⁷⁺ compounds from Re₂⁶⁺ compounds, both of which are examined structurally and electrochemically. [Os₂(hpp) ₄]⁺ is examined to improve upon earlier studies, yielding a model of the g-tensor components with respect to the compound structure.

An additional project included in the dissertation involves the study of an asymmetric trinickel extended metal atom chain. The structural effects of the asymmetry are examined to help elucidate the magnetic behavior that differs significantly from symmetric trinickel extended metal atom chains.