Controlling the Growth of Cs2PbX4 Nanostructures Enhances the Stability of Inorganic Cesium-Based Perovskite Solar Cells for Potential Low Earth Orbit Applications.

Incorporating low-dimensional (LD) materials in perovskite solar cells (PSCs) for interfacial engineering is an effective approach to enhance device performance. However, the growth mechanisms for inorganic LD perovskite nanostructures in cesium-based systems via solution processing are underexplored. This work demonstrates the importance of controlling solvent evaporation dynamics during solution processing to modulate Cs2PbX4 nanomorphology. An evolution of growing Cs2PbX4 nanostructures is demonstrated on CsPbI2Br thin films. Cs2PbX4 nanostructures at CsPbI2Br grain boundaries introduce a passivation effect, improving interfacial quality with the hole transport layer (HTL). Systematic characterization reveals that careful engineering of LD nanostructures strongly impacts the optoelectronic properties of PSCs. Optimized CsPbI2Br/Cs2PbX4 heterostructures enhance the power conversion efficiency (PCE) from an average of 10.8% to 13.5%, achieving a 25% improvement over devices without interfacial engineering. Under a 100 h photovoltaic aging test, the PCE of the control device degraded by 30.7%, whereas the CsCl-treated devices retained 98% of their PCE from the start of the measurement. Post-proton-irradiated PSCs based on Cs2PbX4-modified CsPbI2Br retain up to 96% of their initial PCE of 12.2% after exposure to low Earth orbit-like conditions, maintaining a PCE of 11.7%. In contrast, the control device exhibits significant degradation, with the PCE dropping from 11.5% to 3.1%. These findings deepen our understanding of controlling the morphology of inorganic LD nanomaterials via a solution process. The promising stability of PSCs after interfacial engineering highlights their potential for robust performance under harsh conditions.