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Despite the youthfulness of hybrid halide perovskite solar cells, their efficiencies are currently comparable to commercial silicon and have surpassed quantum‐dots solar cells. Yet, the scalability of these devices is a challenge due to their low reproducibility and stability under environmental conditions. However, the techniques reported to date to tackle such issues recurrently involve the use of solvent methods that would further complicate their transfer to industry. Herein a reliable alternative relaying in the implementation of an ultrathin plasma polymer as a passivation interface between the electron transport layer and the hybrid perovskite layer is presented. Such a nanoengineered interface provides solar devices with increased long‐term stability under ambient conditions. Thus, without involving any additional encapsulation step, the cells retain more than 80% of their efficiency after being exposed to the ambient atmosphere for more than 1000 h. Moreover, this plasma polymer passivation strategy significantly improves the coverage of the mesoporous scaffold by the perovskite layer, providing the solar cells with enhanced performance, with a champion efficiency of 19.2%, a remarkable value for Li‐free standard mesoporous n‐i‐p architectures, as well as significantly improved reproducibility. [ABSTRACT FROM AUTHOR]

Perovskite Solar Cells: Enhanced Stability of Perovskite Solar Cells Incorporating Dopant-Free Crystalline Spiro-OMeTAD Layers by Vacuum Sublimation (Adv. Keywords: organometal halide perovskites; perovskite solar cells; solid state hole conductors; Spiro-OMeTAD; stability; vacuum deposition Organometal halide perovskites, perovskite solar cells, solid state hole conductors, Spiro-OMeTAD, stability, vacuum deposition. [Extracted from the article]

The main handicap still hindering the eventual exploitation of organometal halide perovskite‐based solar cells is their poor stability under prolonged illumination, ambient conditions, and increased temperatures. This article shows for the first time the vacuum processing of the most widely used solid‐state hole conductor (SSHC), i.e., the Spiro‐OMeTAD [2,2′,7,7′‐tetrakis (N,N‐di‐p‐methoxyphenyl‐amine) 9,9′‐spirobifluorene], and how its dopant‐free crystalline formation unprecedently improves perovskite solar cell (PSC) stability under continuous illumination by about two orders of magnitude with respect to the solution‐processed reference and after annealing in air up to 200 °C. It is demonstrated that the control over the temperature of the samples during the vacuum deposition enhances the crystallinity of the SSHC, obtaining a preferential orientation along the π–π stacking direction. These results may represent a milestone toward the full vacuum processing of hybrid organic halide PSCs as well as light‐emitting diodes, with promising impacts on the development of durable devices. The microstructure, purity, and crystallinity of the vacuum sublimated Spiro‐OMeTAD layers are fully elucidated by applying an unparalleled set of complementary characterization techniques, including scanning electron microscopy, X‐ray diffraction, grazing‐incidence small‐angle X‐ray scattering and grazing‐incidence wide‐angle X‐ray scattering, X‐ray photoelectron spectroscopy, and Rutherford backscattering spectroscopy. [ABSTRACT FROM AUTHOR]