Doctor of Philosophy (Ph.D.)
Degree Granting Department
Sarath Witanachchi, Ph.D.
Pritish Mukherjee, Ph.D.
Hariharan Srikanth, Ph.D.
Denis Karaiskaj, Ph.D.
Manh-Huong Phan, Ph.D.
Organolead Halides, BaTiO3 nanoparticles, Ferroelectric Polarization, UV-Vis-NIR Spectroscopy, X-ray Diffraction, Scanning Electron Microscopy, Aerosol Assisted Chemical Vapor Deposition
Organometal halide perovskite absorbers such as methylammonium lead iodide chloride (CH3NH3PbI3-xClx), have emerged as an exciting new material family for photovoltaics due to its appealing features that include suitable direct bandgap with intense light absorbance, band gap tunability, ultra-fast charge carrier generation, slow electron-hole recombination rates, long electron and hole diffusion lengths, microsecond-long balanced carrier mobilities, and ambipolarity. The standard method of preparing CH3NH3PbI3-xClx perovskite precursors is a tedious process involving multiple synthesis steps and, the chemicals being used (hydroiodic acid and methylamine) are quite expensive. This work describes a novel, single-step, simple, and cost-effective solution approach to prepare CH3NH3PbI3-xClx thin ﬁlms by the direct reaction of the commercially available CH3NH3Cl (or MACl) and PbI2. A detailed analysis of the structural and optical properties of CH3NH3PbI3-xClx thin ﬁlms deposited by aerosol assisted chemical vapor deposition is presented. Optimum growth conditions have been identified. It is shown that the deposited thin films are highly crystalline with intense optical absorbance.
Charge carrier separation of these thin films can be enhanced by establishing a local internal electric field that can reduce electron-hole recombination resulting in increased photo current. The intrinsic ferroelectricity in nanoparticles of Barium Titanate (BaTiO3 -BTO) embedded in the solar absorber can generate such an internal field. A hybrid structure of CH3NH3PbI3-xClx perovskite and ferroelectric BTO nanocomposite FTO/TiO2/CH3NH3PbI3-xClx: BTO/P3HT/Cu as a new type of photovoltaic device is investigated. Aerosol assisted chemical vapor deposition process that is scalable to large-scale manufacturing was used for the growth of the multilayer structure. TiO2 and P3HT with additives were used as ETL and HTL respectively. The growth process of the solar absorber layer includes the nebulization of a mixture of PbI2 and CH3NH3Cl perovskite precursors and BTO nanoparticles dissolved in DMF, and injection of the aerosol into the growth chamber and subsequent deposition on TiO2. While high percentage of BTO in the film increases the carrier separation, it also leads to reduced carrier generation. A model was developed to guide the optimum BTO nanoparticle concentration in the nanocomposite films. Characterization of perovskite solar cells indicated that ferroelectric polarization of BTO nanoparticles leads to the increase of the width of depletion regions in the perovskite layer hence the photo current was increased by one order of magnitude after poling the devices. The ferroelectric polarization of BTO nanoparticles within the perovskite solar absorber provides a new perspective for tailoring the working mechanism and photovoltaic performance of perovskite solar cells.
Scholar Commons Citation
Hettiarachchi, Chaminda Lakmal, "Organometal Halide Perovskite Solar Absorbers and Ferroelectric Nanocomposites for Harvesting Solar Energy" (2017). USF Tampa Graduate Theses and Dissertations.