Nanostructured photovoltaic devices for next generation solar cell

As the search for alternative sources of energy other than petroleum continues to expand, solar energy conversion has already been identified as one of the most promising technologies. In the past few years there has been extensive research focused on the next generation solar cells that can exceed the Shockley-Queisser limit (a model that predicts the maximum achievable efficiency for a given material with a given bandgap). Moreover, nanoengineering approaches to enhance solar power conversion efficiency have started to receive considerable interest. Even in the most efficient commercially available solar devices utilizing crystalline silicon, a major portion of the absorbed ultraviolet photon energy is wasted as heat. Furthermore, this heat is detrimental to device reliability. Colloidal nanocrystal quantum dots (NQDs) offer the exciting prospect of simultaneously manipulating device and material structures and processes to enable more efficient solar energy conversion. Most importantly, these colloidal nanocrystal quantum dots are amenable to inexpensive fabrication techniques such as dip coating or spray coating of the constituent nanoscale materials onto various substrates.;This dissertation focuses on the development of nanostructured photovoltaic devices, that exhibit multiple exciton generation, and that exploit the wide absorption spectra enabled by the quantum dots for next generation highly efficient, low cost, solar cells. Firstly, multiple exciton generation and subsequent electrical extraction from a thin film photoconductive device constructed from PbSe NQDs is demonstrated. As an extension of this work, this PbSe NQD photoconductor was used in a tandem structure with a polymer solar cell to demonstrate multiple carrier extraction the application of an external electric field. This structure exhibited improved device durability from UV irradiation due to the self-passivating effect provided by the PbSe layer.;In order to achieve better exciton dissociation and charge transport, novel NQDs with functionalized ligands were developed. This research included the development of an approach to produce predefined patterns of quantum dots and multipod nanocrystals. The technique used optical lithography for direct writing of device structures for optoelectronic and electronic devices as well as the ability to change the ligand properties by using heat treatment. CdSe, CdTe, and PbSe nanocrystals were all functionalized by the incorporation of the functional ligand t-butoxycarbonyl (t-BOC). The ability to modify ligands of spin-casted nanocrystal layers by heating enables the fabrication of multi-layered structures. Moreover, the direct photopatterning of nanocrystal device structures was facilitated by the incorporation of a photo acid generator with the t-BOC functionalized nanocrystals.;Finally, three different approaches that were recently developed to use t-BOC protected NQDs for photovoltaic devices will be discussed. The three types of devices that were developed include: (1) a multi-layered NQD all inorganic heterojunction photovoltaic devices; (2) a Schottky junction solar cell using a metal electrode on a NQD thin film; and (3) a hybrid (NQD/Polymer) bulk heterojunction device. Detailed characterization of these devices demonstrated that the t-BOC protected NQDs can be used to boost device performance (as compared to devices made from NQD with other ligands). This result provides significant advantages for realizing complicated device structures in the future.