Copper complexes, being known to have interesting chemistry, are exploited as photosensitizers and redox shuttles in dye-sensitized solar cells (DSSCs). In the most successful example, using Cu(II/I)(tmby)2 as a redox shuttle achieves a 13.7% power conversion efficiency (PCE) under 1 sun and 34% under 1000 lux. In these systems, however, base additives like 4-tert-butylpyridine (TBP) are shown to undergo ligand exchange reactions with certain Cu2+ centers, resulting in a loss of solution potential and hindering the exploitation of copper redox shuttles to their full potential. In this thesis, an investigation of a new class of copper complexes with sterically crowded ligands is discussed. Uniquely, showing the potential of these complexes to act simultaneously as chromophores and redox shuttles offers the possibility of dramatically higher efficiencies. The role of TBP in ligand exchange and redox reactions is examined, using cyclic voltammetry, UV-Vis absorption spectroscopy, and 1H NMR measurements. In addition, describing the details of this reaction and how it maps onto dye-sensitized solar cell performance as both a chromophore and redox shuttle, along with future directions.In the latter part of this thesis, a novel class of organic single-crystal thin films is explored, advancing the field of optoelectronics by developing highly ordered organic materials. Offering exceptional electronic and optical properties, these single-crystal organic solid crystals are positioned as promising candidates for a range of high-performance optical and electronic devices, paving the way for new applications in next-generation optoelectronic systems and impacting fields such as displays, sensors, and photonic circuits.
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