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In the pursuit of highly efficient perovskite solar cells, spiro‐OMeTAD has demonstrated recorded power conversion efficiencies (PCEs), however, the stability issue remains one of the bottlenecks constraining its commercial development. In this study, we successfully synthesize a novel self‐polymerized spiro‐type interfacial molecule, termed v‐spiro. The linearly arranged molecule exhibits stronger intermolecular interactions and higher intrinsic hole mobility compared to spiro‐OMeTAD. Importantly, the vinyl groups in v‐spiro enable in situ polymerization, forming a polymeric protective layer on the perovskite film surface, which proves highly effective in suppressing moisture degradation and ion migration. Utilizing these advantages, poly‐v‐spiro‐based device achieves an outstanding efficiency of 24.54 %, with an enhanced open‐circuit voltage of 1.173 V and a fill factor of 81.11 %, owing to the reduced defect density, energy level alignment and efficient interfacial hole extraction. Furthermore, the operational stability of unencapsulated devices is significantly enhanced, maintaining initial efficiencies above 90 % even after 2000 hours under approximately 60 % humidity or 1250 hours under continuous AM 1.5G sunlight exposure. This work presents a comprehensive approach to achieving both high efficiency and long‐term stability in PSCs through innovative interfacial design. [ABSTRACT FROM AUTHOR]

Quasi‐2D perovskites have shown great potential in achieving solution‐processed electrically pumped laser diodes due to their multiple‐quantum‐well structure, which induces a carrier cascade process that can significantly enhance population inversion. However, continuous‐wave (CW) optically pumped lasing has yet to be achieved with near‐infrared (NIR) quasi‐2D perovskites due to the challenges in obtaining high‐quality quasi‐2D films with suitable phase distribution and morphology. This study regulates the crystallization of a NIR quasi‐2D perovskite ((NMA)2FAn−1PbnI3n+1) using an 18‐crown‐6 additive, resulting in a compact and smooth film with a largely improved carrier cascade efficiency. The amplified spontaneous emission threshold of the film is reduced from 47.2 to 35.9 µJ cm−2. Furthermore, by combining the film with a high‐quality distributed feedback grating, this study successfully realizes a CW NIR laser of 809 nm at 110 K, with a high Q‐factor of 4794 and a low threshold of 911.6 W cm−2. These findings provide an important foundation for achieving electrically pumped laser diodes based on the unique quasi‐2D perovskites. [ABSTRACT FROM AUTHOR]

In the pursuit of highly efficient perovskite solar cells, spiro-OMeTAD has demonstrated recorded power conversion efficiencies (PCEs), however, the stability issue remains one of the bottlenecks constraining its commercial development. In this study, we successfully synthesize a novel self-polymerized spiro-type interfacial molecule, termed v-spiro. The linearly arranged molecule exhibits stronger intermolecular interactions and higher intrinsic hole mobility compared to spiro-OMeTAD. Importantly, the vinyl groups in v-spiro enable in situ polymerization, forming a polymeric protective layer on the perovskite film surface, which proves highly effective in suppressing moisture degradation and ion migration. Utilizing these advantages, poly-v-spiro-based device achieves an outstanding efficiency of 24.54 %, with an enhanced open-circuit voltage of 1.173 V and a fill factor of 81.11 %, owing to the reduced defect density, energy level alignment and efficient interfacial hole extraction. Furthermore, the operational stability of unencapsulated devices is significantly enhanced, maintaining initial efficiencies above 90 % even after 2000 hours under approximately 60 % humidity or 1250 hours under continuous AM 1.5G sunlight exposure. This work presents a comprehensive approach to achieving both high efficiency and long-term stability in PSCs through innovative interfacial design., (© 2024 Wiley-VCH GmbH.)

Three-dimensional (3D) perovskites have been demonstrated as an effective strategy to achieve efficient light-emitting diodes (LEDs) at high brightness. However, most 3D perovskite LEDs still suffer from serious efficiency roll-off. Here, using FAPbI 3 as a model system, we find that the main reason for efficiency droop and degradation in 3D perovskite LEDs is defects and the ion migration under electrical stress. By introducing bifunctional-molecule 3-chlorobenzylamine additive into the perovskite precursor solution, the detrimental effects can be significantly suppressed through the growth of high crystalline perovskites and defect passivation. This approach leads to bright near-infrared perovskite LEDs with a peak external quantum efficiency of 16.6%, which sustains 80% of its peak value at a high current density of 460 mA cm -2 , corresponding to a high brightness of 300 W sr -1 m -2 . Moreover, the device exhibits a record half-lifetime of 49 h under a constant current density of 100 mA cm -2 .