............................................................................................................................... ii List of Figures .................................................................................................................... vii List of Tables ..................................................................................................................... xiii List of Schemes .................................................................................................................. xvi List of Abbreviations ....................................................................................................... xvii Acknowledgments .............................................................................................................. xx Chapter 1 : Introduction ............................................................................................ 1 1.0: Preface ........................................................................................................................... 1 1.1: Metal Organic Frameworks ........................................................................................ 1 1.1.1: Historical Perspectives .......................................................................................................... 5 1.1.2: First Generation MOFs ......................................................................................................... 7 1.1.3: Second Generation MOFs ................................................................................................... 12 1.1.4: Third Generation MOFs ...................................................................................................... 18 1.2: Molecular Magnetism ................................................................................................ 33 1.2.1: Traditional vs Molecule-based Magnets ............................................................................. 34 1.2.2: Principles of Magnetism ..................................................................................................... 35 1.2.3: Single-Molecule Magnets (SMMs) ..................................................................................... 45 1.3: Introduction to MOLCAS and Post Hartree-Fock Methods.................................. 65 1.3.1: MOLCAS ............................................................................................................................ 65 1.3.2: Introduction to Hartree-Fock Calculations.......................................................................... 66 1.3.3: Post-Hartree-Fock Calculations .......................................................................................... 76 Chapter 2 : Project 1 Synthesis and Characterization of a “Breathing” MOF with a Novel Topology ............................................................................................... 84