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Despite the outstanding electric properties and cost-effectiveness of poly(3,4-ethylenedioxythiophene) (PEDOT) and its derivatives, their performance as hole transport layer (HTL) materials in conventional perovskite solar cells (PSCs) has lagged behind that of widely used spirobifluorene-based molecules or poly(triaryl amine). This gap is mainly from their poor solubility and energy alignment mismatch. In this work, the design and synthesis of a pyrrole-modified HTL (PPr) based on 3,4-propylenedioxythiophene (ProDOT) are presented for efficient and stable PSCs. As a result of the superior defects passivation ability, excellent contact with perovskite, enhanced hole extraction, and high hydrophobicity, the unencapsulated PPr-based PSCs showed the peak PCE of 21.49% and outstanding moisture stability (over 4000 h). This work highlights the potential application of ProDOT-based materials as HTL for PSCs and underscores the importance of the rational design of PEDOT and its derivatives.

2D perovskite (PVSK) single crystals have received significant attention due to their unique optical and optoelectronic properties. However, current synthesis methods face limitations, particularly in large-area fabrication, which remain critical barriers to practical applications. In this study, the synthesis of red/green/purple-blue-colored 2D PVSK nanocrystals over a large area (4-inch wafer) and the fabrication of high-performance photodetector arrays are presented via a facile yet efficient spray-coating approach with a liquid-bridge transport effect. The photodetector array achieves 100% working yield, high photo-responsivity (1.5 × 10 6  A W -1 ) and specific-detectivity (1.1 × 10 16 Jones) with competitive photomapping characteristics. An intelligent vision system for automatic shape recognition is further demonstrated with a recognition rate exceeding 90%. This study provides significant advances in the scalable synthesis of nanoscale 2D PVSK crystals, their integration into large-area optoelectronic devices, and their potential use in artificial-intelligence systems., (© 2025 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Twisted halide perovskite bilayers, a type of moiré material, show square moiré patterns with exciting optical properties. Atomic-scale structure analysis and its correlation with properties are difficult to achieve due to the extreme sensitivity of organic-inorganic halide perovskites to the illuminated electron beam in conventional/scanning transmission electron microscopy. Here, we developed a low-dose exit wave reconstruction methodology with a real-space resolution of one angstrom at ∼50 e/Å 2 , which recovers the phase information on the moiré fringes in CH 3 NH 3 PbI 3 (MAPbI 3 ) twisted perovskite bilayers at atomic scale, enabling detailed structural analysis of defects and corresponding strain distribution in such moiré materials. This work provides an atomic-level understanding of electron beam-sensitive twisted bilayer materials.