Probing Local Heterogeneity in the Optoelectronic Properties of Organic-Inorganic Perovskites Using Fluorescence Microscopy

by Dane Dequilettes

Institution: University of Washington
Year: 2018
Keywords: Fluorescence Microscopy; Nanotechnology; Perovskite; Photoluminescence; Solar Energy; Spectroscopy; Chemistry; Physical chemistry; Materials Science; Chemistry
Posted: 02/01/2018
Record ID: 2215958
Full text PDF: http://hdl.handle.net/1773/40861


Unregulated emission of carbon dioxide and greenhouse gases into our atmosphere has led to an increase in the average global surface air temperature, to a disruption of weather patterns, and to the acidification of oceans all of which threaten the continued prosperity of our race and our planet. The transition to renewable sources of energy is therefore one of, if not the most, important challenge that the 21st century faces. Solar energy is predicted to play a major role in global energy production in the coming century, as the amount of energy hitting the earths surface is far greater than the energy demands of industrialized human activity. Many current photovoltaic technologies show promise in contributing to a large fraction of global energy production, but in order to reach terawatt-scale production the photovoltaic modules will need to be scalable, cheap, and efficient. Perovskite-based photovoltaics hold exceptional potential in contributing to solar energy production. Thus far, the unprecedented rise in power conversion efficiencies over the past few years can be primarily attributed to improvements in film processing and device engineering. Although effective, the fundamental photophysical processes that govern charge generation, transport, recombination, and collection in these materials is still in its infancy. Historically in semiconductor technologies, this understanding has been essential in the rational design of optimized materials. This knowledge appears to be even more critical as perovskite thin films are polycrystalline on the microscale, which suggests that the local structure may determine the optoelectronic quality and device performance on a similar length scale. Prior to these studies, much of the field had focused on bulk spectroscopic measurements to characterize the semiconducting properties of hybrid perovskite thin films. From our contributions as well as many others, microscopy has now given us a window into how this bulk behavior is composed of an ensemble of spatially varying structure and composition, which controls carrier transport and dynamics on the way to carrier extraction and power generation. This understanding has led to some exciting new discoveries on the rational design of materials and is leveraged to deploy chemical passivation techniques to improve the optoelectronic quality of the material, with the ultimate goal of improving photovoltaic power conversion efficiency. Reducing non-radiative recombination in semiconducting materials is a prerequisite for achieving the highest performance in a host of light-emitting and photovoltaic applications. In the first study described herein, we used confocal fluorescence microscopy correlated with scanning electron microscopy to spatially resolve the photoluminescence (PL) decay dynamics from films of nonstoichiometric organic-inorganic perovskites, CH3NH3PbI3(Cl). The PL intensities and lifetimes varied between different grains in the same film, even for films that exhibited long bulk lifetimes. The grain boundaries wereAdvisors/Committee Members: Ginger, David S (advisor).