The Defect Structure and Performance of Methylammonium Lead Trihalide Thin-film Based Photovoltaics
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In order to limit global warming to 1.5-2 °C deployed solar photovoltaic (PV) power must increase from today's 0.228 terawatts to 2-10 terawatts installed by 2030, depending on demand. These goals require increasing manufacturing capacity, which, in turn, requires lowering the cost of electricity produced by PV. However, high demand scenarios will require greater cost reductions in order to make PV generated electricity <i> as competitive </i> as it needs to be to enable this growth. It is unclear whether established PV technologies — silicon, CdTe, GaAs, or CuInxGa1-xSe2 — can achieve the necessary breakthroughs in efficiency and price. A newer technology known as the 'perovskite solar cell' (PSC) has recently emerged as promising contender. <br> In the last seven years the efficiency of PSCs increased by the same amount covered by established technologies in the last thirty. However, PSCs suffer from chemical instability under operating conditions and hysteresis in current-voltage measurements used to characterize power output. Characterizing the defect structures formed by this material and how they interact with device performance and degradation may allow stabilization of PSCs. To that end, this work investigates defects in perovskite solar cells, the impact of these defects on performance, and the effect of alloying and degradation on the electronically active defect structure. Chapter I gives a brief introduction, motivating research in solar cells generally and perovskites in particular as well as introducing some challenges the technology faces. Chapter II gives some background in semiconductors and the device physics of solar cells. Chapter III introduces the performance and defect characterization methods employed. Chapter IV discusses results of these measurements on methylammonium lead triiodide cells correlating defects with device performance. Chapter V applies the some of the same techniques to a series of CH3NH3Pb(I1-xBrx)3 based perovskites aged for up to 2400 hours to explore the impact of alloying and aging on the defect structure. Chapter VI discusses implications for perovskite development and directions for future research. <br> This dissertation includes previously published co-authored material.