Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.030
Publication date: 18th December 2023
Organic-inorganic metal halide perovskites have emerged as attractive materials for solar cells with power-conversion efficiencies of single-junction devices now exceeding 26%. However, instabilities arising from facile ionic migration may still pose challenges to long-term deployment. One issue that still limits the implementation of silicon-perovskite tandem cells in particular, is the peculiar mechanisms underlying detrimental halide segregation in mixed iodide-bromide lead perovskites with desirable electronic band gaps near 1.8eV.[1-5] We reveal that, surprisingly, halide segregation results in negligible impact to the THz charge-carrier mobilities.[2] However, remarkably fast, picosecond charge funnelling into the narrow-bandgap I-rich domains leads to enhanced radiative recombination.[3]Performance losses in photovoltaic devices may therefore potentially be mitigated by deployment of careful light management strategies. We further demonstrate[3] how a combination of simultaneous in-situ photoluminescence and X-ray diffraction measurements is able to demonstrate clear differences in compositional and optoelectronic changes associated with halide segregation in MAPb(Br0.5I0.5)3 and FA0.83Cs0.17Pb(Br0.4I0.6)3 films. While MAPb(Br0.5I0.5)3 exhibits rearrangement of halide ions only in localized volumes of perovskite, FA0.83Cs0.17Pb(Br0.4I0.6)3 lacks such low-barrier ionic pathways and is, consequently, more stable against halide segregation. However, under prolonged illumination, it exhibits a considerable ionic rearrangement throughout the bulk material, which may be triggered by an initial demixing of A-site cations, altering the composition of the bulk perovskite and reducing its stability against halide segregation.[4] We further explore the influence of a hole-transport layer, necessary for a full device. We show that top coating FA0.83Cs0.17Pb(Br0.4I0.6)3 perovskite films with a poly(triaryl)amine (PTAA) hole-extraction layer surprisingly leads to suppression of halide segregation because photogenerated charge carriers are rapidly trapped at interfacial defects that do not drive halide segregation.[4] In addition, we examine temperature- and light-induced reversal of halide segregation.[5] We show that increasing temperature from 125K kinetically enhances halide segregation up to 290K, but higher temperatures hinder it owing to entropic remixing. Increasing the incident light intensity can also induce remixing, but we show this effect to be transient and derive from local heating.[5]
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