Yingdong Xia

Magnetron‐sputtered nickel oxide (NiO _x ) has emerged as a stable and efficient hole transport layer (HTL) for high‐performance inverted perovskite solar cells (PSCs) due to its high carrier mobility, excellent stability, and compatibility with large‐scale manufacturing. However, the limited crystallinity of sputtered NiO _x films and interfacial mismatch with perovskites still restrict device efficiency. Here, we present a synergistic strategy that integrates sputtering temperature optimization with bilayer molecular modification (Me‐4PACz/PEACl) for interfacial passivation. By tuning the substrate temperature during NiO _x sputtering, its optoelectronic properties were effectively enhanced, while sequential deposition of Me‐4PACz and phenethylammonium chloride (PEACl) layers further regulated the buried perovskite interface and passivated defects. As a result, the optimized PSCs achieved a champion power conversion efficiency (PCE) of 23.37%. The unencapsulated devices retained over 90% of their initial PCE after 1500 h of storage under an inert N ₂ atmosphere, highlighting their excellent operational stability. Importantly, benefiting from the compatibility of magnetron sputtering with scalable screen‐printing processes, large‐area devices (1 cm ² ) were successfully fabricated, underscoring the scalability and industrial potential of this integrated approach.

Carbazole‐based self‐assembled monolayers (SAMs) are widely used in high‐performance perovskite solar cells (PSCs); however, single‐component SAMs often suffer from incomplete coverage on FTO substrates and weak interactions with the perovskite layer, leading to interfacial defects and crystallization stress. Herein, we develop a synergistic interface engineering strategy by introducing a phosphine‐based molecule, bis(4‐trifluoromethylphenyl)(4‐carboxyphenyl)phosphine (TFMP), to construct a ternary cooperative interface (Co‐SAM@TFMP) based on a co‐adsorbed self‐assembled monolayer (Co‐SAM) composed of [4‐(3,6‐dimethyl‐9H‐carbazol‐9‐yl)butyl]phosphonic acid (Me‐4PACz) and [4‐(9'‐phenyl‐9H,9'H‐[3,3'‐bicarbazol]‐9‐yl)butyl]phosphonic acid (4PABCz). In this system, the phosphonic and carboxylic acid groups are firmly anchored to the substrate, improving the integrity of the interfacial coverage. At the buried interface, TFMP acts as a molecular bridge by coordinating with Pb ²⁺ and stabilizing FA ⁺ , thereby suppressing interfacial defects. Furthermore, this cooperative interface alleviates crystallization stress during perovskite film growth through flexible molecular segments, promoting the formation of uniform and highly crystalline films. Ultimately, the optimized inverted PSCs achieved a power conversion efficiency (PCE) of 26.78%, and the unencapsulated devices retained 93.7% of their initial PCE after continuous operation at the maximum power point for 1200 h. This work offers a general and effective strategy for interface modulation toward high‐performance perovskite solar cells and related optoelectronic devices.

This review highlights recent advances in highly efficient and stable inverted PSCs and discusses key directions for achieving large-area fabrication and enhanced stability to accelerate commercialization.

A multifunctional ionic liquid enables anion-competition-regulated Pb ²⁺ coordination, directing the growth of oriented porous PbI ₂ frameworks for scalable, high-efficiency, and stable perovskite solar cells.

Phase-pure α-formamidinium lead iodide (α-FAPbI ₃ ) perovskites that exclude additional cations or anions (for example, methylammonium (MA ⁺ ), Cs ⁺ , or Br ⁻ ) hold great promise for high-efficiency and thermally stable perovskite solar cells.

Pentyl propionate (PAAC) weakens DMF–Pb ²⁺ coordination via dipole interactions, moderating nucleation and crystallization, enabling high-quality films and devices with a power conversion efficiency of 24.06%.