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Abstract:

The deposition of large ammonium cations onto perovskite surfaces to passivate defects and reduce contact recombination has enabled exceptional efficiency and stability in perovskite solar cells. These ammonium cations can either assemble as a thin molecular layer at the perovskite surface or induce the formation of a low-dimensional (usually two-dimensional) perovskite capping layer on top of the three-dimensional perovskite. The formation of these two different structures is often overlooked by researchers, although they impact differently on device operation. In this Review, we seek to distinguish between these two passivation layers. We consider the conditions needed for the formation of low-dimensional perovskite and the electronic properties of the two structures. We discuss the mechanisms by which each method improves photovoltaic efficiency and stability. Finally, we summarize the knowledge gaps that need to be addressed to better understand and optimize ammonium cation-based passivation strategies.

Abstract:

Next-generation light-emitting applications such as displays and optical communications require judicious control over emitted light, including intensity and angular dispersion. To date, this remains a challenge as conventional methods require cumbersome optics. Here, we report highly directional and enhanced electroluminescence from a solution-processed quasi-2-dimensional halide perovskite light-emitting diode by building a device architecture to exploit hybrid plasmonic-photonic Tamm plasmon modes. By exploiting the processing and bandgap tunability of the halide perovskite device layers, we construct the device stack to optimise both optical and charge-injection properties, leading to narrow forward electroluminescence with an angular full-width half-maximum of 36.6° compared with the conventional isotropic control device of 143.9°, and narrow electroluminescence spectral full-width half-maximum of 12.1 nm. The device design is versatile and tunable to work with emission lines covering the visible spectrum with desired directionality, thus providing a promising route to modular, inexpensive, and directional operating light-emitting devices.

Abstract:

Perovskite solar cells (PSCs) with an "inverted" architecture are a key pathway for commercializing this emerging photovoltaic technology due to the better power conversion efficiency (PCE) and operational stability as compared to the "normal" device structure. Specifically, PCEs of the inverted PSCs have exceeded 25% owing to the development of improved self-assembled molecules (SAMs)^1-5 and passivation strategies^6-8. Nevertheless, poor wettability and agglomerations of SAMs^9-12 will cause interfacial losses, impeding further improvement in PCE and stability. Herein, we report on molecular hybrid at the buried interface in inverted PSCs by co-assembling a multiple carboxylic acid functionalized aromatic compound of 4,4',4''-nitrilotribenzoicacid (NA) with a popular SAM of [4-(3,6-dime-thyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz) to improve the heterojunction interface. The molecular hybrid of Me-4PACz with NA could substantially improve the interfacial characteristics. The resulting inverted PSCs demonstrated a record-certified steady-state efficiency of 26.54%. Crucially, this strategy aligns seamlessly with large-scale manufacturing, achieving the highest certified PCE for inverted mini-modules at 22.74% (aperture area: 11.1 cm²). Our device also maintained 96.1% of its initial PCE after more than 2,400 hours of 1-sun operation in ambient air.

Abstract:

Further improvements in perovskite solar cells require better control of ionic defects in the perovskite photoactive layer during the manufacturing stage and their usage. Here we report a living passivation strategy using a hindered urea/thiocarbamate bond Lewis acid–base material (HUBLA), where dynamic covalent bonds with water and heat-activated characteristics can dynamically heal the perovskite to ensure device performance and stability. Upon exposure to moisture or heat, HUBLA generates new agents and further passivates defects in the perovskite. This passivation strategy achieved high-performance devices with a power conversion efficiency (PCE) of 25.1 per cent. HUBLA devices retained 94 per cent of their initial PCE for approximately 1,500 hours of ageing at 85 degrees Celsius in nitrogen and maintained 88 per cent of their initial PCE after 1,000 hours of ageing at 85 degrees Celsius and 30 per cent relative humidity in air.