Some of the material in is restricted to members of the community. By logging in, you may be able to gain additional access to certain collections or items. If you have questions about access or logging in, please use the form on the Contact Page.
The exploration of new paradigms for micro- and nanoelectronics has engendered several exciting new research fields including molecular electronics and spintronics. Two essential ingredients of the device structures are materials and interfaces. The overarching theme of this dissertation is the study of the (spin-dependent) electronic states and transport in novel magnetic materials and through molecular interfaces. These experiments are necessary first steps in ascertaining potential utilities in molecular electronic and spintronics applications. More importantly for this thesis, the materials and hybrid device structures provide a fertile ground for studying basic physics of magnetism, magnetotransport, and spin transport. In this dissertation, various techniques of superconducting spectroscopy have been used to investigate the spin-dependent electronic density of states of the thiol/Au molecular interface and the ferromagnetic semimetal EuB6. In addition, a fresh analysis of the electronic transport properties of EuB6 reveals a new type of nonlinear Hall effect intimately related to its magnetic state and culminates in a model that offers excellent quantitative understanding of the data and appears applicable to a wide varieties of magnetic materials. In order to directly probe possible induced magnetism at the thiol-gold interface, spin polarized tunneling measurements were performed on planar tunnel junctions incorporating a molecular monolayer of mercaptohexadecanoic acid [HS(CH2)15COOH] (MHA) between aluminum and gold electrodes. The Zeeman resolved tunneling spectra yield no measurable spin polarization at the thiol-gold interface, contrary to the expectations from the reported induced giant magnetic moments at the interface. On the other hand, variations in the resistance of the fabricated tunnel junctions with changing environmental conditions were consistently observed. A systematic investigation revealed that the effect is directly linked to the interaction of water molecules with the carboxylate groups of the MHA monolayer at the AlOx surface. Analyses of the I-V characteristics produce compelling evidence for significant modifications of the tunnel barrier height of the AlOx upon adsorption of the MHA monolayer, and subsequently by the reaction of water molecules with the carboxylate group at the AlOx surface. The results demonstrate that environmental effects could significantly impact the electron transport even in molecular junctions of macroscopic dimensions and closed architecture. Andreev reflection spectroscopy measurements performed on junctions consisting of EuB6 single crystals and lead electrodes clearly demonstrated that EuB6 is not a half metal with a fully spin polarized Fermi surface. Instead, the measured spin polarization values range from 47% to 65%. Analyses based on the measured spin polarization together with Fermi surface and transport measurements lead to a quantitatively consistent picture in agreement with a semimetallic band structure with a substantial band splitting for the valence band only in the ferromagnetic phase. Moreover, the analyses also indicate a semimetallic band structure with localized holes in the paramagnetic phase and a delocalization of the holes near ferromagnetic ordering. Our studies on EuB6 provide important clarification of its spin dependent band structure. Hall effect and magnetoresistance measurements were also performed on EuB6 single crystals. The data are consistent with previous reports. However, we offer a new analysis of the Hall effect which has led to significant new insights. An unusual change in the Hall resistivity slope with increasing magnetic field was observed in the paramagnetic phase. The change in Hall resistivity slope was found to occur at a universal critical magnetization at all temperatures. A two-component model based on a picture of intrinsic (non-chemical) electronic/magnetic inhomogeneities and coalescing of a phase with higher conductivity and degree of magnetic ordering was proposed to fit the observed Hall effect. Excellent quantitative agreement was obtained and with this model all the Hall resistivity data were scaled onto a single curve. Significantly, this model and picture were found to offer consistent description of the nonlinear Hall effect in a diverse group of magnetic materials including the mixed valence perovskites and the heavy fermion metal YbRh2Si2. The results indicate that this may be a common form of Hall effect associated with percolative magnetic phase transitions.