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Between Structure and Performance in Halide Perovskites for Photovoltaic Applications: the Role of Defects

, , and . (2018)cite arxiv:1809.10949Comment: PhD thesis.

Abstract

My study is about Halide Perovskites (HaPs) and focuses the fundamental structural, chemical and dielectric properties of HaPs in reference to their PV-related properties. * I present my main research model: HaP single-crystals - their growth and characterization; * I start by exploring the bond nature of HaPs using Nanoindentation and Solid-State NMR techniques. * I explore the 'deformation potential' of the structure and show that its low and positive value in HaPs strongly suggests a pronounced 'defect tolerance'. * I explore the scattering mechanism of charges in the soft and highly polarizable system such as HaPs, and show that its low mobility (relative to other heteropolar systems) is fundamental and cannot be improved. I also show that a positive 'deformation potential' (so the valence band is 'anti-bonding', where a system should promote 'defect-tolerance') is something that is common to other highly polarizable systems, such as AgX, and Pb-chalcogenides. * I explore the chemistry of the system and show that HaPs can easily break to constituents, but also easily be made by the same constituents, suggesting a low activation energy for annealing process to take care even at RT. This RT annealing can promote 'self-healing' at ~second to ~minute time-scale, which we clearly observe. We find 'entropic-stabilization' to be very important in 'self-healing' processes of that kind. * I explore the importance of symmetry breaking in the HaP structure, which can induce a polar - and thus Ferroelectric - structure. We conclude that Ferroelectricity is not a fundamental property of HaPs, since it doesn't exist in MAPbBr3, but only in MAPbI3 - as proven unambiguously - and what is present in MAPbI3 is in doubt important for photovoltaics, when using them at RT or above. Due to compression, if you find a low-quality figure you want- please email me.

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[1809.10949] Between Structure and Performance in Halide Perovskites for Photovoltaic Applications: the Role of Defects

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