Effects of Electron-Vibron Coupling in Single-Molecule Magnet Transport Junctions Using a Hybrid Density Functional Theory and Model Hamiltonian Approach

Recent experiments have shown that junctions consisting of individual single-molecule magnets (SMMs) bridged between two electrodes can be fabricated in three-terminal devices, and that the characteristic magnetic anisotropy of the SMMs can be affected by electrons tunneling through the molecule. Vibrational modes of the SMM can couple to electronic charge and spin degrees of freedom, and this coupling also influences the magnetic and transport properties of the SMM. The effect of electron-vibron coupling on transport has been extensively studied in small molecules, but not yet for junctions of SMMs. The goals of this thesis will be two-fold: to present a novel approach for studying the effects of this electron-vibron coupling on transport through SMMs that utilizes both density functional theory calculations and model Hamiltonian construction and analysis, and to present a software framework based on this hybrid approach for the simulation of transport across user-defined SMMs. The results of these simulations will indicate a characteristic suppression of the current at low energies that is strongly dependent on the overall electron-vibron coupling strength and number of molecular vibrational modes considered.