Indium tin oxide serve a critical function in many organic devices, such as organic light emitting diodes and organic photovoltaics. To optimize the performances of these devices, it is desirable to tune the interface between the indium tin oxide and the next functional layer of these devices. A common surface modification of transparent conductive oxides is through the use of self-assembled monolayers. This methodology enables a simultaneously tuning of the properties and performance of this interface, including the surface energy, work function and durability of the transparent conductive oxide. Phosphonic acid and silane based monolayers have been extensively studied and used in devices for their ability to tune the interfacial properties of transparent conductive oxide. Herein, alcohol based monolayers are first demonstrated on transparent conductive oxide surfaces. The electrochemical and chemical stabilities of alcohol based monolayers, as well as changes in the optical properties of the Indium tin oxide as a function of their stability were evaluated in comparison to more traditional routes of surface modification, such as through the use of silanes and phosphonic acid based monolayers. The tunability of both work function and surface energy of the modified Indium tin oxide were also determined for assessing their electronic properties.

Phosphonic acids are known to bind strongly to a variety of metal oxide surfaces. Phosphonic acids were designed in order to impart specific properties to the surface of a range of metal oxides upon formation of a monolayer. A large number of novel phosphonic acids were synthesized and fully characterized. The binding of phosphonic acids to the surface of several metal oxides, such as indium tin oxide (ITO) and barium titanate, was studied in detail and determined to be a mixture of bidentate and tridentate binding modes. The modification of several key surface properties of ITO by phosphonic acid modification was also studied. The work function of ITO could be increased or decreased with respect to unmodified ITO by controlling the dipole of phosphonic acids bound to the surface. Additionally, the surface energy could be substantially lowered by attaching phosphonic acids with non-polar terminal functional groups to the ITO surface. The ability to control these surface properties resulted in organic light-emitting diodes (OLEDs) which showed superior lifetimes and stability with respect to OLEDs incorporating ITO without a phosphonic acid monolayer. In addition, the binding of phosphonic acids to a number of other oxides, such as zinc oxide and zeolites, was also studied.

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This thesis addresses the problem of improving the alignment of carbon nanotubes (CNTs) in transistor applications, taking a unique approach using iptycenes acting as molecular tweezers in combination with a liquid crystal solvent. As part of a project to test the effectiveness of a multi-step method, the so-called Alignment Relay Technique (ART), this work contributed evidence for the selectivity and stability of ART, as well as providing the first proof-of-concept that ART can be used to create CNT field-effect transistors (FETs). The thesis effectively explains and illustrates the chemical synthesis of the tweezers, the concept and actualization of the technique, the various factors observed to influence deposition and selectivity, along with material fabrication using both photolithography and electron beam lithography. This research advances knowledge of transistors and expands the applications of small organic molecules in the field of materials science. Particular highlights of this thesis include: an extensive review of ART, its advantages, and limitations; development of new material chemistry methods for the optimization of semiconducting CNT selectivity; and a comprehensive exploration of fabrication and characterization of CNTFETs for future applications.

A practical guidebook illustrating the applications of spectroelectrochemistry to the understanding of redox reactions through identification of their intermediaries and products.