Several solvothermal synthetic methods have been developed to produce novel low-dimensional magnetic materials and determine their structure-properties relationships. Two main classes of compounds were investigated, including iron selenides and transition metal formate-chlorides.

Chapter 2 details the development of the first solution-based synthetic route to superconducting iron (II) selenide. Samples were found to retain superconducting properties only when air and water were rigorously excluded from the synthesis.

Chapter 3 presents the synthesis, structure, and magnetic properties of two new mixed-valence compounds with infinite ∞¹(FeSe ₂) tetrahedral chains separated by Fe-amine complexes. The use of different Fe-amine complexes allows for tuning of the magnetic properties without changing the general structural motif.

Chapters 4 and 5 report the first members of the transition metal chloride-formate family of compounds, which contain linear zig-zag chains of octahedrally coordinated metal atoms linked by μ₂-Cl and syn-syn formate bridges. These compounds order antiferromagnetically and exhibit metamagnetic transitions.

Chapter 6 describes a related set of transition metal formate-chloride compounds that are comprised of helical chains of edge-sharing M²⁺ -centered octahedra. These compounds undergo 3D ferrimagnetic ordering at low temperature, and are rare examples of homospin topological ferrimagnets.