Engineering Earth-Abundant Colloidal Plasmonic and Semiconductor Nanomaterials for Solar Energy Harvesting and Detection Applications

Colloidal nanomaterials have shown intriguing optical and electronic properties, making them important building blocks for a variety of applications, including photocatalysis, photovoltaics, and photodetectors. Their morphology and composition are effective tuning knobs for achieving desirable spectral characteristics for specific applications. In addition, they can be synthesized using solution-processed methods which possess the advantages of low cost, facile fabrication, and compatibility with building flexible devices. There is an ongoing quest for better colloidal materials with superior properties and high natural abundance for commercial viability. This thesis focuses on three such materials classes and applications: 1) studying the photophysical properties of earth-abundant plasmonic alumionum nanoparticles, 2) tailoring the optical profiles of semiconductor quantum dot solar cells with near-infrared sensitivity, and 3) using one-dimensional nanostructures for photodetector applications. A variety of analytical techniques and simulations are employed for characterization of both the morphology and optical properties of the nanostructures and for evaluating the performance of nanomaterial-based optoelectronic devices. The first experimental section of this thesis consists of a systematic study of electron relaxation dynamics in solution-processed large aluminum nanocrystals. Transient absorption measurement are used to obtain the important characteristic relaxation timescales for each thermalization process. We show that several of the relevant timescales in aluminum differ from those in analogous noble metal nanoparticles and proposed that surface modification could be a useful tool for tuning heat transfer rates between the nanostructures and solvent. Further systematic studies on the relaxation dynamics in aluminum nanoparticles with tunable sizes show size-dependent phonon vibrational and damping characteristics that are influenced by size polydispersity, surface oxidation, and the presence of organic capping layers on the particles. These studies are significant first steps in demonstrating the feasibility of using aluminum nanomaterials for efficient photocatalysis. The next section summarizes studies on the design and fabrication of multicolored PbS-based quantum dot solar cells. Specifically, thin film interference effects and multi-objective optimization methods are used to generate cell designs with controlled reflection and transmission spectra resulting in programmable device colors or visible transparency. Detailed investigations into the trade-off between the attainable color or transparency and photocurrent are discussed. The results of this study could be used to enable solar cell window-coatings and other controlled-color optoelectronic devices. The last experimental section of thesis describes work on using 1D antimony selenide nanowires for flexible photodetector applications. A one-pot solution-based synthetic method is developed for producing a molecular ink which allows fabrication of devices on flexible substrates. Thorough characterization of the nanowire composition and morphology are performed. Flexible, broadband antimony selenide nanowire photodetectors are fabricated and show fast response and good mechanical stability. With further tuning of the nanowire size, spectral selectivity should be achievable. The excellent performance of the nanowire photodetectors is promising for the broad implementation of semiconductor inks in flexible photodetectors and photoelectronic switches