| Summary: | <p> 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.</p><p> 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.</p><p> Chapter 3 presents the synthesis, structure, and magnetic properties of two new mixed-valence compounds with infinite ∞<sup>1</sup>(FeSe<sub> 2</sub>) 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.</p><p> 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 μ<sub>2</sub>-Cl and <i>syn-syn</i> formate bridges. These compounds order antiferromagnetically and exhibit metamagnetic transitions.</p><p> Chapter 6 describes a related set of transition metal formate-chloride compounds that are comprised of helical chains of edge-sharing M<sup>2+ </sup>-centered octahedra. These compounds undergo 3D ferrimagnetic ordering at low temperature, and are rare examples of homospin topological ferrimagnets. </p><p>
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