Molecular spintronics aims to enhance current electronic devices and create new ones by merging molecular electronics with spintronics. A key focus is on exploring molecular magnets for device applications, particularly single-molecule magnets (SMMs) and hybrid-molecular magnets, which serve as potential building blocks for spintronic devices like spin-transistors and spin-valves. Successful device fabrication hinges on understanding the complex interactions between molecules and surfaces. This dissertation investigates these interactions through experimental approaches conducted in ultra-high vacuum to mitigate contamination. The structural, electronic, and magnetic properties of these systems were analyzed using scanning tunneling microscopy (STM) and spectroscopy (STS). The interaction between SMMs and surfaces was specifically examined by depositing Ni4 on Au(111), where Ni4 features a cubane Ni II 4 (3Cl)4 core responsible for its magnetic properties, protected by thioether-functionalized organic ligands. Experiments using XPS and STM indicated significant ligand detachment during adsorption, although the magnetic core appeared structurally intact. Attempts to desorb the detached ligands and image the magnetic core via in-situ post-annealing were unsuccessful, leading instead to core decomposition and surface reconstruction. This study proposes new strategies to prevent ligand detachment in future experiments.
