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Inverted (p-i-n) perovskite solar cells (PSCs) have experienced remarkable advancements in recent years, which is largely attributed to the development of novel hole-transport layer (HTL) self-assembled monolayer (SAM) materials. Methoxy (MeO-) groups are typically introduced into SAM materials to enhance their wettability and effectively passivate the perovskite buried interface. However, MeO-based SAM materials exhibit a mismatch in highest occupied molecular orbital (HOMO) levels with perovskite layer due to the strong electron-donating capability of methoxy group. In this work, we introduced a methylthio (MeS-) substituent that is superior to methoxy as a highly versatile self-assembled molecular design strategy. As a soft base, sulfur atom forms a stronger Pb-S bond than oxygen. Additionally, within the CbzPh series of SAM materials, MeS-CbzPh demonstrates a more optimal HOMO level and enhanced hole transport properties. Consequently, the MeS-CbzPh HTL based device achieved an impressive power conversion efficiency (PCE) of 26.01 % and demonstrated high stability, retaining 93.3 % efficiency after 1000 hours of maximum power point tracking (MPPT). Moreover, in comparison with the commonly used 4PACz-based SAM molecular series, MeS-4PACz also exhibited the best performance among its peers. Our work provides valuable insights for the molecular design of SAM materials, offering a highly versatile functional substituent group., (© 2024 Wiley-VCH GmbH.)

The device performance of deep-blue perovskite light-emitting diodes (PeLEDs) is primarily constrained by low external quantum efficiency (EQE) especially poor operational stability. Herein, we develop a facile strategy to improve deep-blue emission through rational interface engineering. We innovatively reported the novel electron transport material, 4,6-Tris(4-(diphenylphosphoryl)phenyl)-1,3,5-triazine (P-POT2T), and utilized a sequential wet-dry deposition method to form the homogenic gradient interface between electron transport layer (ETL) and perovskite surface. Unlike previous reports that achieved carrier injection balance by inserting new interlayers, our strategy not only passivated uncoordinated Pb 2+ in the perovskite via P=O functional groups but also reduced interfacial carrier recombination without introducing new interfaces. Additionally, this strategy enhanced the interface contact between the perovskite and ETL, significantly boosting device stability. Consequently, the fabricated deep-blue PeLEDs delivered an EQE exceeding 5 % (@ 460 nm) with an exceptional halftime extended to 31.3 minutes. This straightforward approach offers a new strategy to realize highly efficient especially stable PeLEDs., (© 2024 Wiley-VCH GmbH.)

Achieving high-efficiency perovskite solar cells (PSCs) hinges on the precise control of the perovskite film crystallization process, often improved by the inclusion of additives. While dimethyl sulfoxide (DMSO) is traditionally used to manage this process, its removal from the films is problematic. In this work, methyl phenyl sulfoxide (MPSO) was employed instead of DMSO to slow the crystallization rate, as MPSO is more easily removed from the perovskite structure. The electron delocalization associated with the benzene ring in MPSO decreases the electron density around the oxygen atom in the sulfoxide group, thus reducing its interaction with PbI 2 . This strategy not only sustains the formation of a crystallization-slowing intermediate phase but also simplifies the elimination of the additive. Consequently, the optimized PSCs achieved a leading power conversion efficiency (PCE) of 25.95 % along with exceptional stability. This strategy provides a novel method for fine-tuning perovskite crystallization to enhance the overall performance of photovoltaic devices., (© 2024 Wiley-VCH GmbH.)