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The self‐assembled hole transporting molecules (SAHTMs) bearing anchoring groups have been established as the hole transporting layers (HTLs) for highly efficient p–i–n perovskite solar cells (PSCs), yet their stability and engineering at the molecular level remain challenging. A topological design of highly anisotropic aligned SAHTM‐based HTLs for operationally stable PSCs that exhibit exceptional solar‐to‐electric power conversion efficiencies (PCEs) is demonstrated. The judiciously designed multifunctional self‐assembled molecules comprise the donor–acceptor subunit for hole transporting and the phosphonic acid group for anchoring, realizing face‐on π‐stacking parallel to the transparent conductive oxide substrate. The high affinity of SAHTMs to the multi‐crystalline perovskite thin film benefits passivating the perovskite buried interface, strengthening interfacial contact while facilitating interfacial hole transfer. Consequently, highly efficient p–i–n PSC devices are obtained with a champion PCE of 23.24% and outstanding operational stability toward various environmental factors including long‐term full sunlight soaking at evaluated temperatures. Perovskite solar modules with a champion efficiency approaching 20% are also fabricated for an active device area above 17 cm2. [ABSTRACT FROM AUTHOR]

Long‐term stability has become the major obstacle for the successful large‐scale application of perovskites devices. Owing to the ionic nature of metal‐halide perovskites, the interfacial ion diffusion can induce irreversible degradation under operational conditions, which presents a great challenge to realize stable perovskite solar modules. Here, a diphenylphosphine oxide compound, ethane‐1,2‐diylbis(diphenylphosphine oxide) (DPPO) is introduced to coordinate with lead iodide and form a cross‐linked 1D Pb3I6‐DPPO (1D‐PbI2) complex. These judiciously designed cross‐linked nonionic low‐dimensional lead halide/organic adducts can passivate the defects of perovskite while acting as a robust ion diffusion barrier, thus significantly improving the electronic quality and intrinsic stability of perovskite films. As a result, high‐performance inverted (p‐i‐n) solar modules with a champion efficiency approaching 19% (a certified stabilized efficiency of 17.8%) for active device areas above 17 cm2 without the use of antisolvents, accompanied by outstanding operational stability under heat stress and continuous illumination are achieved. [ABSTRACT FROM AUTHOR]

[Display omitted] • PNCs-radical core/shell structure was prepared by P -type organic radical polymer. • This structure improves the stability of PNCs with charge transfer processes. • The stable PNCs-radical core/shell complex demonstrate superb reduction ability. • This strategy could promote the performance of PNCs based n-i-p solar cells. Balancing the stability and interfacial charge transfer (CT) ability of perovskite nanocrystals (PNCs) are the most challenging issue confronting their practical application in photoelectrochemistry (PEC) fields. Here, an efficient surface capping strategy is introduced relying on a set of air-stable nitroxide-based organic radical polymers with well-matched energy levels towards CsPbBr 3 nanocrystals. The native ligand oleyl amine and oleic acid were readily replaced by radical polymers because of their high-affinity properties. The resulting radical polymer coated PNCs exhibit exceptional tolerance to water, thermal, and UV illumination with remarkable CT processes. The versatility and immense practical utility of such stable PNCs-radical core/shell structure are showcased by the halogen exchange between PNCs/radical and aryl chlorides at ambient temperature, demonstrating superb reduction ability of this complex. Besides, this strategy was also employed to improve the power conversion efficiency and stability of PNCs based solar cells. This approach imparts exceptional photoelectrochemical stability and catalytic activity to the nanocrystals with excellent interfacial CT efficiency. [ABSTRACT FROM AUTHOR]

[Display omitted] • TPA-BA modification results in improved interfacial energy band alignment. • TPA-BA modification reduces interfacial chemical reactivity. • The TPA-BA-modified devices achieve a power conversion efficiency of 22.25%. • TPA-BA-based devices remained stable after illumination and thermal aging tests. Nickel oxide (NiO x) is one of the most promising inorganic hole transport layers for perovskite solar cells (PSCs) due to its low cost, high hole mobility, and superior stability. However, the mismatched energy level and undesirable chemical reaction at the NiO x /perovskite interface limit the performance of NiO x -based PSCs. Herein, a p- type semiconductor TPA-BA is explored to modify the NiO x /perovskite interface and form an intermediate hole transport layer (HTL) between NiO x and perovskite for efficient and efficient stable PSCs. This molecule comprises triphenylamine and carboxyl function groups, which can be anchored on the NiOx surface and facilitate the hole transfer between the perovskite and NiO x layer by minimizing the interfacial band energy offset. Furthermore, the bi-layered NiO x HTL exhibited reduced chemical reactivity at NiO x /perovskite interface, which would otherwise lead to detrimental perovskite degradation. Thus, a champion PSC device with an open-circuit voltage value up to 1.15 V and a power conversion efficiency of 22.25% was demonstrated-a high value for NiO x -based PSCs. More importantly, the intermediated HTL modified PSCs exhibit significantly improved device stability compared with un-modified PSCs, retaining over 90 % of their initial efficiencies after 1000-h continuous operation under 1 sun illumination and thermal aging at 85 °C respectively. This work renders the promise of TPA-BA as the intermediated HTL in between p -type metal oxide and perovskite for optoelectronic applications. [ABSTRACT FROM AUTHOR]