Ever-increasing global energy demand and a diminishing fossil fuel supply have prompted the development of technologies for sustainable energy production. Solar photovoltaic (PV) devices have huge potential for energy harvesting and production since the sun delivers more energy to the earth in one hour than the global population consumes in one year. The solar cell industry is now dominated by silicon PV devices. The cost of silicon modules has decreased substantially over the past two decades and the number of installed silicon PV devices has increased dramatically. There remains a need for emerging solar technologies that can harvest the untapped portion of the solar spectrum and can be integrated on flexible and curved surfaces. This thesis focuses on colloidal quantum dot (CQD) PV devices. CQDs are nanoparticles fabricated using a low-temperature and cost-effective solution technique. These materials suffer from a high density of surface traps derived from the large surface-to-volume ratio of CQD nanoparticles, combined with limited carrier mobility. These result in a short carrier diffusion length, a main limiting factor in CQD solar cell performance. This thesis seeks to address the poor diffusion length in lead sulfide (PbS) CQD films and pave the way for new applications for CQD PV devices in infrared solar harvesting and waste heat recovery. A two-fold reduction in surface trap density is demonstrated using molecular halide treatment. Iodine molecules introduced prior to the film formation replace the otherwise unpassivated surface sulfur atoms. This results in a 35% increase in the diffusion length and enables charge extraction over thicker active layer leading to the world's most efficient CQD PV devices from June 2015 to July 2016 with the certified power conversion efficiency of 9.9%. This represents a 30% increase over the best-certified PCE (7.5%) prior to this thesis. The colloidal engineering highlighted herein enables infrared (IR) solar harvesting for the first time. Addition of short bromothiol ligands during the synthesis significantly reduces the agglomeration of 1 eV bandgap CQDs and maintains efficient charge extraction into the selective electrodes. The devices can augment the performance of the best silicon cells by 7 power points where 0.8 additive power points are demonstrated experimentally. A tailored solution exchanged process developed for 1 eV bandgap CQDs results in air-stable IR PV devices with improved manufacturability. The process utilizes a tailored combination of lead iodide (PbI2) and ammonium acetate for the solution exchange and hexylamine + MEK as the final solvent to yield solar thick films with the filtered (1100 nm and beyond) performance of 0.4%. This thesis pushes the limit of CQD device applications to waste heat recovery. I demonstrate successful harvesting of low energy photons emitted from a hot object by designing and developing the first solution-processed thermophotovoltaic devices. These devices are comprised of 0.7 eV bandgap CQDs that successfully harvest photons emitted from an 800°C heat source.
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