Despite the incredible progress made, the highest efficiency perovskite solar cells are still restricted to small areas (<1 cm 2 ). In large part, this stems from a poor understanding of the widespread spatial heterogeneity in devices. Conventional techniques to assess heterogeneities can be time consuming, operate only at microscopic length scales, and demand specialized equipment. We overcome these limitations by using luminescence imaging to reveal large, millimeter-scale heterogeneities in the inferred electronic properties. We determine spatially resolved maps of "charge collection quality", measured using the ratio of photoluminescence intensity at open and short circuit. We apply these methods to quantify the inhomogeneities introduced by a wide range of transport layers, thereby ranking them by suitability for upscaling. We reveal that top-contacting transport layers are the dominant source of heterogeneity in the multilayer material stack. We suggest that this methodology can be used to accelerate the development of highly efficient, large-area modules, especially through high-throughput experimentation.

Lead halide perovskites (LHPs) have emerged as an excellent class of semiconductors for next-generation solar cells and optoelectronic devices. Tailoring physical properties by fine-tuning the lattice structures has been explored in these materials by chemical composition or morphology. Nevertheless, its dynamic counterpart, phonon-driven ultrafast material control, as contemporarily harnessed for oxide perovskites, has not yet been established. Here, we use intense THz electric fields to obtain direct lattice control via nonlinear excitation of coherent octahedral twist modes in hybrid CH 3 NH 3 PbBr 3 and all-inorganic CsPbBr 3 perovskites. These Raman-active phonons at 0.9 to 1.3 THz are found to govern the ultrafast THz-induced Kerr effect in the low-temperature orthorhombic phase and thus dominate the phonon-modulated polarizability with potential implications for dynamic charge carrier screening beyond the Fröhlich polaron. Our work opens the door to selective control of LHP’s vibrational degrees of freedom governing phase transitions and dynamic disorder.

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