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Understanding the fundamental properties of buried interfaces in perovskite photovoltaics is of paramount importance to the enhancement of device efficiency and stability. Nevertheless, accessing buried interfaces poses a sizeable challenge because of their non‐exposed feature. Herein, the mystery of the buried interface in full device stacks is deciphered by combining advanced in situ spectroscopy techniques with a facile lift‐off strategy. By establishing the microstructure–property relations, the basic losses at the contact interfaces are systematically presented, and it is found that the buried interface losses induced by both the sub‐microscale extended imperfections and lead‐halide inhomogeneities are major roadblocks toward improvement of device performance. The losses can be considerably mitigated by the use of a passivation‐molecule‐assisted microstructural reconstruction, which unlocks the full potential for improving device performance. The findings open a new avenue to understanding performance losses and thus the design of new passivation strategies to remove imperfections at the top surfaces and buried interfaces of perovskite photovoltaics, resulting in substantial enhancement in device performance.

It is common practice in the lead halide perovskite solar cell field to add a small molar excess of lead iodide (PbI 2 ) to the precursor solution to increase the device performance. However, recent reports have shown that an excess of PbI 2 can accelerate performance loss. In addition, PbI 2 is photoactive (band gap ∼2.3 eV), which may lead to parasitic absorption losses in a solar cell. Here we show that devices using small quantities of excess PbI 2 exhibit better device performance as compared with stoichiometric devices, both initially and for the duration of a stability test under operating conditions, primarily by enhancing the charge extraction. However, the photolysis of PbI 2 negates the beneficial effect on charge extraction by leaving voids in the perovskite film and introduces trap states that are detrimental for device performance. We propose that although excess PbI 2 provides a good template for enhanced performance, the community must continue to seek other additives or synthesis routes that fulfill the same beneficial role as excess PbI 2 , but without the photolysis that negates these beneficial effects under long-term device operation.

Stable but not quite cubic The black, photoactive phase of formamidinium (FA) perovskites, which is usually stabilized by cation alloying to avoid the formation of inactive hexagonal phases, is assumed to be cubic. High-resolution microscopy studies by Doherty et al . using nanoscale probes revealed that these FA-rich phases are not cubic but rather undergo slight tilting (by two degrees) of the octahedra. Black phases can have localized regions of hexagonal phases that nucleate degradation. Surface-bound ethylenediaminetetraacetic acid stabilized the tilted phase of pure FA lead triiodide against environmental degradation. —PDS

Halide perovskites of the form ABX 3 have shown outstanding properties for solar cells. The highest reported compositions consist of mixtures of A-site cations methylammonium (MA), formamidinium (FA) and cesium, and X-site iodide and bromide ions, and are produced by solution processing. However, it is unclear whether solution processing will yield sufficient spatial performance uniformity for large-scale photovoltaic modules or compatibility with deposition of multilayered tandem solar cell stacks. In addition, the volatile MA cation presents long-term stability issues. Here, we report the multisource vacuum deposition of FA 0.7 Cs 0.3 Pb(I 0.9 Br 0.1 ) 3 perovskite thin films with high-quality morphological, structural, and optoelectronic properties. We find that the controlled addition of excess PbI 2 during the deposition is critical for achieving high performance and stability of the absorber material, and we fabricate p-i-n solar cells with stabilized power output of 18.2%. We also reveal the sensitivity of the deposition process to a range of parameters, including substrate, annealing temperature, evaporation rates, and source purity, providing a guide for further evaporation efforts. Our results demonstrate the enormous promise for MA-free perovskite solar cells employing industry-scalable multisource evaporation processes.

Understanding the nanoscopic chemical and structural changes that drive instabilities in emerging energy materials is essential for mitigating device degradation. The power conversion efficiency of halide perovskite photovoltaic devices has reached 25.7% in single junction and 29.8% in tandem perovskite/silicon cells 1,2 , yet retaining such performance under continuous operation has remained elusive 3 . Here, we develop a multimodal microscopy toolkit to reveal that in leading formamidinium-rich perovskite absorbers, nanoscale phase impurities including hexagonal polytype and lead iodide inclusions are not only traps for photo-excited carriers which themselves reduce performance 4,5 , but via the same trapping process are sites at which photochemical

The fabrication of multidimensional organometallic halide perovskite via a low-pressure vapor-assisted solution process is demonstrated for the first time. Phenyl ethyl-ammonium iodide (PEAI)-doped lead iodide (PbI ) is first spin-coated onto the substrate and subsequently reacts with methyl-ammonium iodide (MAI) vapor in a low-pressure heating oven. The doping ratio of PEAI in MAI-vapor-treated perovskite has significant impact on the crystalline structure, surface morphology, grain size, UV-vis absorption and photoluminescence spectra, and the resultant device performance. Multiple photoluminescence spectra are observed in the perovskite film starting with high PEAI/PbI ratio, which suggests the coexistence of low-dimensional perovskite (PEA MA Pb I ) with various values of n after vapor reaction. The dimensionality of the as-fabricated perovskite film reveals an evolution from 2D, hybrid 2D/3D to 3D structure when the doping level of PEAI/PbI ratio varies from 2 to 0. Scanning electron microscopy images and Kelvin probe force microscopy mapping show that the PEAI-containing perovskite grain is presumably formed around the MAPbI perovskite grain to benefit MAPbI grain growth. The device employing perovskite with PEAI/PbI = 0.05 achieves a champion power conversion efficiency of 19.10% with an open-circuit voltage of 1.08 V, a current density of 21.91 mA cm , and a remarkable fill factor of 80.36%.

Large datasets are now ubiquitous as technology enables higher-throughput experiments, but rarely can a research field truly benefit from the research data generated due to inconsistent formatting, undocumented storage or improper dissemination. Here we extract all the meaningful device data from peer-reviewed papers on metal-halide perovskite solar cells published so far and make them available in a database. We collect data from over 42,400 photovoltaic devices with up to 100 parameters per device. We then develop open-source and accessible procedures to analyse the data, providing examples of insights that can be gleaned from the analysis of a large dataset. The database, graphics and analysis tools are made available to the community and will continue to evolve as an open-source initiative. This approach of extensively capturing the progress of an entire field, including sorting, interactive exploration and graphical representation of the data, will be applicable to many fields in materials science, engineering and biosciences.