Electrochemical cell devices are increasingly being sought for energy conversion and storage applications due to their high efficiencies and their potential for operating free of greenhouse gas (GHG) emissions. Solid Acid Electrochemical Cells (SAECs), which most commonly employ CsH2PO4 (CDP) as the electrolyte component, are uniquely suited to meet the...
A fundamental materials science question is “why and how will this material form?” The experimental,computation, and time resources necessary to answer this question consume significant resources due to the
predominantly trial-and-error based approaches common in materials research. This dissertation reintroduces
a number of fundamental thermodynamics-based tools for the study of...
The demand for low cost, unconventional electronics requires new materials with unique characteristics that the traditionally used silicon-based technologies cannot provide. Metal oxide semiconductors, such has amorphous indium gallium zinc oxide (a-IGZO), have made impressive strides as alternatives to amorphous silicon for electronics applications. However, to achieve the full potential...
Metal–Organic Frameworks (MOFs) is a class of material comprising organic linkers and inorganic, metal-ion-containing nodes, with diverse functionalities and wide-range of applications. Because of their porous nature and functional nodes and linkers, they are competent candidates for gas storage, separation, catalysis, and so on. Most MOFs, however, are intrinsically insulating,...
Mixed-dimensional heterojunctions between two-dimensional (2D) materials and organic semiconductors is a rapidly growing field. This is motivated by the promise of leveraging the extraordinary properties of 2D materials with the synthetic tunability and reconfigurability of organic electronics, allowing the realization of new physics or devices that are not possible in...
Renewable energy technology, more so than ever before, is critical to the survival of humanity. For decades, concentrated efforts into designing and developing such novel devices resulted in the innovation of solar-driven photovoltaics that were competitive with nonrenewable alternatives. This thesis explores the dynamic behavior of alternative material candidates that...
The Controlled, Site-Isolated Synthesis of Polyelemental Nanostructures in Polymer Nanoreactors Pengcheng Chen Polyelemental nanoparticles are an attractive class of materials due to their potential applications, which span the fields of catalysis, plasmonics, electronics, magnetics, targeted drug delivery, and bio-imaging. However, conventional synthetic methods for such structures are limited, especially when...
Wireless power strategies are critical to system level implementation of bio-integrated devices. To achieve mechanically robust, manufacturable systems, batteries are often integrated as an on-board power source to support sensing, wireless communication and signal conditioning. Unfortunately, most sources of battery power use hazardous and environmentally harmful materials, which frustrate incorporation...
Organic semiconductors are an active area of research with great promise for delivering next generation electronics and clean energy technologies. As the field matures, understanding the connection between molecular structure, materials’ properties, and device performance will be critical in finding the right material for an intended application. An effective strategy...
The continuing increase in atmospheric CO2 to concentrations exceeding 400 ppm has attracted considerable attention from both scientists and policymakers. Industrial fossil fuel consumption generates a significant amount of CO2 emissions, and in particular, energy-intensive molecular separations that require thermal processes, such as distillation, drying, or evaporation, are responsible for...
Increasing industrialization and the resulting negative environmental impacts highlight the need to develop alternative renewable energy sources. The Sun is a massive source and organic solar cells are a growing field of study. As new materials are synthesized, the efficiencies of organic solar cells continue to grow, but without an...
One of the grand challenges in materials chemistry and nanochemistry is the development of functional materials through ordered, hierarchical structures using synthetic building blocks. Nature has done this through evolution of molecular components such as nucleic acids, saccharides, lipids, amino acids, and inorganic crystals. The precise spatial positioning of these...
Two-dimensional (2D) hybrid halide perovskites have been the response to their exciting but woefully unstable 3D counterparts. These 2D perovskites have been shown to have respectable stabilities as photovoltaic absorbers, yet they lag behind the 3D perovskites in terms of efficiency. With the need to catch up to the efficiencies...
Part I: Design of Photo-Responsive Molecules towards Biomedical ApplicationsThe use of light to control systems provides numerous advantages such as spatiotemporal precision, non-invasive penetration, and precise energy input. Specifically, molecules that undergo photoinduced cleavage, photoremovable protecting groups (PPGs) have emerged as an active area of research due to their broad...
The idea that structure determines the properties of a material is a powerful concept in chemistry and in all fields in which chemistry is important, including engineering, medicine, and materials science. My research aims to better understand the structure-property relationships of a class of materials known as metal–organic frameworks (MOFs)....
Industrial processes heavily rely on catalysts to control product selectivity and lower energy barriers required for chemical transformations. Catalysts are most commonly solid heterogeneous catalysts that facilitate separations from reaction mixtures and enhance recyclability. Heterogeneous catalysts used in industrial processes exhibit efficacious results, but in certain instances drawing structure-function relationships...
Continuous and coordinated materials discovery efforts have amassed a wealth of knowledge concerning many general classes of materials. The number of known phases of all structure-types, however, is far less than number of possible materials dictated by the elements on the periodic table. Recently, with improved computational abilities and well-developed...
As the interest in rational synthesis for solid-state materials accelerates, there is an urgent need to understand the design principles concealed within these reactions. In situ material synthesis provides such an avenue to not only uncover these assembling rules, but also for finding new materials even in seemingly familiar phase...
Metallic conductivity and broken inversion symmetry were long thought to be contraindicated properties, under the assumption that long-range Coulombic interactions (screened by free charge carriers) were necessary for coordinated polar displacements. Within the past decade, the discovery of polar metals has prompted a rethinking of the relationship between metallicity and...
This thesis describes the synthesis and photophysical characterization of low-dimensionalmaterials—including thin-film semiconductors, colloidal quantum dots, and molecules—with the
broader motivation of integrating them into mixed-dimensional heterostructures with novel
responses to external stimuli. Due to their high surface area to volume ratio and incomplete
dielectric screening, mixed-dimensional heterostructures have high sensitivity...