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Abstract While the challenges associated with the stability of metal halide perovskites are well known and intensely studied, variability in electronic properties represents an equally significant, yet seldom studied, challenge that could potentially slow or inhibit the commercial viability of these systems. In this work, the contactless characterization technique time‐resolved microwave conductivity (TRMC) is used to quantify the variability in electronic properties of the prototypical perovskite, methylammonium lead iodide (MAPbI3) both between different samples, and at different locations within the same sample. Using scanning electron microscopy (SEM) and a quasi‐automated image‐analysis strategy, it is possible to evaluate the metrics of heterogeneity in surface microstructure and correlate them with the electronic properties as obtained by TRMC. Substantial intra‐sample and inter‐sample variation is observed in the mobility‐yield product in samples prepared following differing protocols, and in samples prepared following identical protocols.more » « less
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Hempel, Hannes; Savenjie, Tom_J; Stolterfoht, Martin; Neu, Jens; Failla, Michele; Paingad, Vaisakh_C; Kužel, Petr; Heilweil, Edwin_J; Spies, Jacob_A; Schleuning, Markus; et al (, Advanced Energy Materials)Abstract Mobilities and lifetimes of photogenerated charge carriers are core properties of photovoltaic materials and can both be characterized by contactless terahertz or microwave measurements. Here, the expertise from fifteen laboratories is combined to quantitatively model the current‐voltage characteristics of a solar cell from such measurements. To this end, the impact of measurement conditions, alternate interpretations, and experimental inter‐laboratory variations are discussed using a (Cs,FA,MA)Pb(I,Br)3halide perovskite thin‐film as a case study. At 1 sun equivalent excitation, neither transport nor recombination is significantly affected by exciton formation or trapping. Terahertz, microwave, and photoluminescence transients for the neat material yield consistent effective lifetimes implying a resistance‐free JV‐curve with a potential power conversion efficiency of 24.6 %. For grainsizes above ≈20 nm, intra‐grain charge transport is characterized by terahertz sum mobilities of ≈32 cm2V−1s−1. Drift‐diffusion simulations indicate that these intra‐grain mobilities can slightly reduce the fill factor of perovskite solar cells to 0.82, in accordance with the best‐realized devices in the literature. Beyond perovskites, this work can guide a highly predictive characterization of any emerging semiconductor for photovoltaic or photoelectrochemical energy conversion. A best practice for the interpretation of terahertz and microwave measurements on photovoltaic materials is presented.more » « less
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