Once Aviram and Ratner mathematically showed that electronics could be constructed from organic molecules, 1 great interest has been expressed in the development of nanoscale devices containing organics. A tempting application for such devices has been the continued miniaturization of transistors, in an effort to maintain Moore's law. State-of-the-art transistors rely on gated silicon-based circuitry which, when reduced to sufficiently small sizes, fail to prevent electrons from transporting across the gate via quantum tunneling effectively rendering the transistor useless. While this has not slowed research into the development of smaller and smaller silicon chips, molecular electronics provides an attractive alternative. For one, devices designed with organic molecules exist, by their very nature, at the atomic scale allowing researchers to build from the ground up rather than scale current technology down. Secondly, the exact control of molecular structure yields unique features and quantum phenomena beyond what silicon alone could provide. The selective control of a molecule's frontier molecular orbitals has led to the development of molecular junctions capable of filtering spin current. Such capabilities have applications in spintronic technology, for example writing to a solid-state drive. Others have investigated the use of molecular junctions as sensors. Furthermore, single-molecule junctions offer a testbed to study chemical reactions at the single-molecule level. Equally importantly, single-molecule junctions are ideal systems to investigate the fundamental nature of current at the nanoscale. Despite these advantages, challenges prevent the widespread adoption of molecular electronics. Discrepancies between experimental investigations and theoretical modeling constitute a major hurdle to understanding and controlling charge transport at the nanoscale. Experimentally, the current-voltage characteristics of molecular junctions are studied via mechanical-controlled-break junctions, a technique that utilizes a piezometer to bend a thin gold wire to the point of breaking to form electrodes with atomically thin tips, allowing the gas-phase target molecules to bind between the two electrodes, and tracing the conductance of the resulting junction. Or a solution of the target molecules is brought in contact with an electrode metal, such as a gold surface, and a scanning tunneling microscope (STM) tip is rapidly smashed into the gold surface, forming and breaking the junction. These experimental methods necessarily require the repeated breaking and formation of the molecular junction resulting in a distribution of conductance rather than a single well-defined value leading to further discrepancy between experiment and theory.