Non-radiative recombination loss at the hole transport layer (HTL)/perovskite interface in the narrow-bandgap (NBG) subcell constrains the power-conversion efficiency (PCE) of all-perovskite tandem solar cells 1,2. Minimizing charge recombination at the buried interface of lead-tin (Pb-Sn) based NBG perovskite solar cells have proven particularly challenging, as conventional long-chain amine-based passivation strategies often induce carrier transport losses, thereby limiting both the fill factors (FF) and short-circuit current density (Jsc) 3-5. Here, we developed a dipolar passivation strategy that reduces the trap density at the buried interface of mixed Pb-Sn perovskite while simultaneously enabling precise energy level alignment at the HTL/perovskite interface. This dipolar-induced passivation enhances ohmic contact, facilitating efficient hole injection into the HTL and repelling electrons from the HTL/Pb-Sn perovskite interface. This approach extends the carrier diffusion length to 6.2 μm and enables a substantial enhancement in the PCE of Pb-Sn perovskite solar cells, achieving 24.9% along with an open-circuit voltage (Voc) of 0.911 V, a Jsc of 33.1 mA cm-2 and a high FF of 82.6%. Furthermore, the dipolar passivation effectively mitigates contact losses in the NBG subcell induced by the interconnecting layer of tandem devices, contributing to an outstanding PCE of 30.6% (certified stabilized 30.1%) in all-perovskite tandem solar cells.

Amines are among the most common functional groups in bioactive molecules1. Despite this prevalence, conventional means of converting aromatic amines rely heavily on diazonium intermediates2, which pose significant safety risks due to the explosive nature of these salts3,4. Here, we report a direct deaminative strategy through the formation of N-nitroamines, allowing the direct conversion of inert aromatic C-N bonds into an array of other functional groups, C-X (C-Br, C-Cl, C-I, C-F, C-N, C-S, C-Se, C-O) and C-C bonds. This operationally simple, general protocol establishes a unified strategy for one-pot deaminative cross-couplings by integrating deaminative functionalization with transition-metal-catalyzed arylation, thereby streamlining synthesis and late-stage functionalization. The key advantages of this transformation over other deaminative functionalization methods lies in its versatility across nearly all classes of medicinally relevant heteroaromatic amines, as well as electronically and structurally diverse aniline derivatives, regardless of the position of the amino group. Mechanistic studies, supported by both experimental observations and theoretical analysis, suggest that the aryl cation equivalent reactivity of N-nitroamines is generally favoured in this deaminative process. This study highlights the significant potential of the direct deamination approach in synthetic chemistry, offering a safer alternative to the traditionally explosive and hazardous aryldiazonium chemistry.

Metal halide perovskites with remarkable optoelectronic properties have become a competitive candidate for supporting the efficiency progression of photovoltaics. As the latest record on power conversion efficiency (PCE) of research-cells being comparable to the commercialized silicon cells1-3, the industrialization of perovskite solar cells (PSCs) is on the horizon4,5. Most high-efficiency inverted perovskite solar cells using self-assembled molecules (SAMs) face the challenges due to their aggregation and hydrophobicity. Here we report a "SAM-in-matrix" strategy to distribute partial SAMs into a stable matrix of tris(pentafluorophenyl)borane, which could break the original molecular stacking-induced aggregation. 2D lattice Monte Carlo simulation and experimental results reveal that such strategy can form efficient charge transport channels. This SAM-in-matrix hole transport layer (HTL)-based devices demonstrate universally higher efficiencies for various SAMs with compact surface coverage, decent conductivity, and greatly reduced buried nanovoids. Moreover, this strategy shows prominent applicational potential for scalable production. The SAM-in-matrix HTL on FTO/NiOx substrate facilitates the formation of large-area perovskite films with good crystalline quality and enhanced conductivity of NiOx. 1 m × 2 m large-area perovskite solar module is thus achieved with a certified record efficiency of 20.05%.