Flexible Indoor Perovskite Solar Cells by In Situ Bottom-Up Crystallization Modulation and Interfacial Passivation.

A robust perovskite-buried interface is pivotal for achieving high-performance flexible indoor photovoltaics as it significantly influences charge transport and extraction efficiency. Herein, a molecular bridge strategy is introduced utilizing sodium 2-cyanoacetate (SZC) additive at the perovskite-buried interface to simultaneously achieve in situ passivation of interfacial defects and bottom-up crystallization modulation, resulting in high-performance flexible indoor photovoltaic applications. Supported by both theoretical calculations and experimental evidences, it illustrates how SZCs serve as molecular bridges, establishing robust bonds between SnO2 transport layer and perovskite, mitigating oxygen vacancy defects and under-coordinated Pb defects at interface during flexible fabrication. This, in turn, enhances interfacial energy level alignment and facilitates efficient carrier transport. Moreover, this in situ investigation of perovskite crystallization dynamics reveals bottom-up crystallization modulation, extending perovskite growth at the buried interface and influencing subsequent surface recrystallization. This results in larger crystalline grains and improved lattice strain of the perovskite during flexible fabrication. Finally, the optimized flexible solar cells achieve an impressive efficiency exceeding 41% at 1000 lux, with a fill factor as high as 84.32%. The concept of the molecular bridge represents a significant advancement in enhancing the performance of perovskite-based flexible indoor photovoltaics for the upcoming era of Internet of Things (IoT).

Biocompatible Metal-Free Perovskite Membranes for Wearable X-ray Detectors.

Halide perovskites are emerging as promising materials for X-ray detection owing to their compatibility with flexible fabrication, cost-effective solution processing, and exceptional carrier transport behaviors. However, the challenge of removing lead from high-performing perovskites, crucial for wearable electronics, while retaining their superior performance, persists. Here, we present for the first time a highly sensitive and robust flexible X-ray detector utilizing a biocompatible, metal-free perovskite, MDABCO-NH4I3 (MDABCO = methyl-N'-diazabicyclo[2.2.2]octonium). This wearable X-ray detector, based on a MDABCO-NH4I3 thick membrane, exhibits remarkable properties including a large resistivity of 1.13 × 1011 Ω cm, a high mobility-lifetime product (µ-τ) of 1.64 × 10-4 cm2 V-1, and spin Seebeck effect coefficient of 1.9 nV K-1. We achieve a high sensitivity of 6521.6 ± 700 µC Gyair-1 cm-2 and a low detection limit of 77 nGyair s-1, ranking among the highest for biocompatible X-ray detectors. Additionally, the device exhibits effective X-ray imaging at a low dose rate of 1.87 µGyair s-1, which is approximately one-third of the dose rate used in regular medical diagnostics. Crucially, both the MDABCO-NH4I3 thick membrane and the device showcase excellent mechanical robustness. These attributes render the flexible MDABCO-NH4I3 thick membranes highly competitive for next-generation, high-performance, wearable X-ray detection applications.

Defect Passivation Refinement in Perovskite Photovoltaics: Achieving Efficiency over 45% under Low-Light and Low-Temperature Dual Extreme Conditions.

Perovskite photovoltaics have emerged as the most promising candidates for next-generation light-to-electricity technology. However, their practical application still suffers from energy loss induced by intrinsic defects within the perovskite lattice. Here, a refined defect passivation in perovskite films is designed, which shows a multi-interaction mechanism between the perovskite and passivator. Interestingly, a shift of molecular bonding is observed upon cooling down the film, leading to a stronger passivation of iodine/formamidine vacancies. Such mechanism on device under low-light and low-temperature conditions is further leveraged and a record efficiency over 45% with durable ambient stability (T90 > 4000 h) is obtained. The pioneer application of perovskite solar cells in above dual extreme conditions in this work reveals the key principles of designing functional groups for the passivators, and also demonstrates the capability of perovskites for diverse terrestrial energy conversion applications in demanding environments such as polar regions and outer space.

Interfacial Engineering for Efficient Low-Temperature Flexible Perovskite Solar Cells.

Photovoltaic technology with low weight, high specific power in cold environments, and compatibility with flexible fabrication is highly desired for near-space vehicles and polar region applications. Herein, we demonstrate efficient low-temperature flexible perovskite solar cells by improving the interfacial contact between electron-transport layer (ETL) and perovskite layer. We find that the adsorbed oxygen active sites and oxygen vacancies of flexible tin oxide (SnO2 ) ETL layer can be effectively decreased by incorporating a trace amount of titanium tetrachloride (TiCl4 ). The effective defects elimination at the interfacial increases the electron mobility of flexible SnO2 layer, regulates band alignment at the perovskite/SnO2 interface, induces larger perovskite crystal growth, and improves charge collection efficiency in a complete solar cell. Correspondingly, the improved interfacial contact transforms into high-performance solar cells under one-sun illumination (AM 1.5G) with efficiencies up to 23.7 % at 218 K, which might open up a new era of application of this emerging flexible photovoltaic technology to low-temperature environments such as near-space and polar regions.

Crystallization Control for Ambient Printed FA-Based Lead Triiodide Perovskite Solar Cells.

Upscalable printing of high-performance and stable perovskite solar cells (PSCs) is highly desired for commercialization. However, the efficiencies of printed PSCs lag behind those of their lab-scale spin-coated counterparts owing to the lack of systematic understanding and control over perovskite crystallization dynamics. Here, the controlled crystallization dynamics achieved using an additive 1-butylpyridine tetrafluoroborate (BPyBF4 ) for high-quality ambient printed α-formamidinium lead triiodide (FAPbI3 ) perovskite films are reported. Using in situ grazing-incidence wide-angle X-ray scattering and optical diagnostics, the spontaneous formation of α-FAPbI3 from precursors during printing without the involvement of  Î´-FAPbI3 is demonstrated. The addition of BPyBF4 delays the crystallization onset of α-FAPbI3 , enhances the conversion from sol-gel to perovskite, and reduces stacking defects during printing. Therefore, the altered crystallization results in fewer voids, larger grains, and less trap-induced recombination loss within printed films. The printed PSCs yield high power conversion efficiencies of 23.50% and 21.60% for a 0.09 cm-2 area device and a 5 cm × 5 cm-area module, respectively. Improved device stability is further demonstrated, i.e., approximately 94% of the initial efficiency is retained for over 2400 h under ambient conditions without encapsulation. This study provides an effective crystallization control method for the ambient printing manufacture of large-area high-performance PSCs.

Manipulating the Formation of 2D/3D Heterostructure in Stable High-Performance Printable CsPbI3 Perovskite Solar Cells.

Manipulating the formation process of the 2D/3D perovskite heterostructure, including its nucleation/growth dynamics and phase transition pathway, plays a critical role in controlling the charge transport between 2D and 3D crystals, and consequently, the scalable fabrication of efficient and stable perovskite solar cells. Herein, the structural evolution and phase transition pathways of the ligand-dependent 2D perovskite atop the 3D surface are revealed using time-resolved X-ray scattering. The results show that the ligand size and shape have a critical influence on the final 2D structure. In particular, ligands with smaller sizes and more reactive sites tend to form the n = 1 phase. Increasing the ligand size and decreasing the reactive sites promote the transformation from 3D to n = 3 and n < 3 phases. These findings are useful for the rational design of the phase distribution in 2D perovskites to balance the charge transport and stability of the perovskite films. Finally, solar cells based on ambient-printed CsPbI3 with n-butylammonium iodide treatment achieve an improved efficiency of 20.33%, which is the highest reported value for printed inorganic perovskite solar cells.

Controlling Phase Transition toward Future Low-Cost and Eco-friendly Printing of Perovskite Solar Cells.

Perovskite solar cells (PSCs) have grown increasingly popular over the past few years and are considered to be game-changers in the energy conversion market. It has became vital to transfer the deep understanding of the perovskite film formation process during lab-scale fabrication to large-scale production. Complex phase transition during film formation has been revealed by in situ strategies. However, there is still debate which phase transition is the right route for a future scalable approach. Herein, we briefly summarize perovskite crystallization during scalable printing processes. The critical information about the intermediates involved in phase transition from precursors to perovskite crystals are discussed because it deeply impacts the morphology of printed films. Finally, important strategies to control phase transition and challenges toward future low-temperature and eco-friendly printing of perovskite solar cells are proposed. The information provided by this Perspective will assist the screening and development of the perovskite phase transition for future cost-efficient printed perovskite panels.