Room Temperature Crystallized Phase-Pure α-FAPbI3 Perovskite with In-Situ Grain-Boundary Passivation.

Energy loss in perovskite grain boundaries (GBs) is a primary limitation toward high-efficiency perovskite solar cells (PSCs). Two critical strategies to address this issue are high-quality crystallization and passivation of GBs. However, the established methods are generally carried out discretely due to the complicated mechanisms of grain growth and defect formation. In this study, a combined method is proposed by introducing 3,4,5-Trifluoroaniline iodide (TFAI) into the perovskite precursor. The TFAI triggers the union of nano-sized colloids into microclusters and facilitates the complete phase transition of α-FAPbI3 at room temperature. The controlled chemical reactivity and strong steric hindrance effect enable the fixed location of TFAI and suppress defects at GBs. This combination of well-crystallized perovskite grains and effectively passivated GBs leads to an improvement in the open circuit voltage (Voc) of PSCs from 1.08 V to 1.17 V, which is one of the highest recorded Voc without interface modification. The TFAI-incorporated device achieved a champion PCE of 24.81%. The device maintained a steady power output near its maximum power output point, showing almost no decay over 280 h testing without pre-processing.

Intermediate Phase Free α-FAPbI3 Perovskite via Green Solvent Assisted Perovskite Single Crystal Redissolution Strategy.

Perovskite single-crystal redissolution (PSCR) strategy is highly desired for efficient formamidinium lead triiodide (FAPbI3 ) perovskite photovoltaics with enhanced phase purity, improved film quality, low trap-state density, and good stability. However, the phase transition and crystallization dynamics of FAPbI3 remain unclear in the PSCR process compared to the conventional fabrication from the mixing of precursor materials. In this work, a green-solvent-assisted (GSA) method is employed to synthesize centimeter-sized α-FAPbI3 single crystals, which serve as the high-purity precursor to fabricate perovskite films. The α-FAPbI3 PSCR strategy facilitates direct α-phase formation and inhibits the complex intermediate phases monitored by in situ grazing-incidence wide-angle X-ray scattering. Moreover, the α-phase stability is prolonged due to the relaxation of the residual lattice strain through the isotropic orientation phase growth. Consequently, the GSA-assisted PSCR strategy effectively promotes crystallization and suppresses non-radiative recombination in perovskite solar cells, which boosts the device efficiency from 22.08% to 23.92% with significantly enhanced open circuit voltage. These findings provide deeper insight into the PSCR process in terms of its efficacy in phase formation and lattice strain release. The green low-cost solvent may also offer a new and ideal solvent candidate for large-scale production of perovskite photovoltaics.

Green Solvent Polishing Enables Highly Efficient Quasi-2D Perovskite Solar Cells.

Preferred crystalline orientation at the surface of quasi-2D organic-inorganic halide perovskites is crucial to promote vertical carrier transport and interface carrier extraction, which further contribute to device efficiency and stability in photovoltaic applications. However, loose unoriented and defective surfaces are inevitably formed in the crystallization process, especially with the introduction of bulky organic cations into the quasi-2D perovskites. Here, a facile and effective surface polishing method using a natural-friendly green solvent, 2,2,2-trifluoroethanol, is proposed to reconstruct the surface. After solvent polishing, the randomly oriented phases containing trap sites on the surface are successfully removed, and the compact vertical-oriented phases underneath are revealed with less defectiveness and better smoothness, which greatly facilitates carrier transport and interfacial charge extraction. Consequently, the green solvent polished devices show a boosting efficiency of 18.38% with a high open-circuit voltage of 1.21 V. The devices also show improved storage and operational stability.

Synergy of Block Copolymers and Perovskites: Template Growth through Self-Assembly.

Block copolymers (BCPs) have been widely used as templates to prepare nanostructures over the past few decades. Ordered nanostructures can be formed after microphase segregation of BCPs. In this context, the newly emerging BCP-templated perovskites, in which the perovskite crystal growth has been confined within a self-assembled BCP nanostructure due to the interaction between the polymer block and the cation of the perovskite, have shown profound optical performance and environmental stability. Considering the promising performance of BCP-templated perovskites, this Perspective comprehensively reviews recent works in which BCPs are used as templates with three-dimensional perovskites and perovskite quantum dots, and their performance and stability are thoroughly discussed. Lastly, their potential applications in optoelectronics and biology are discussed.

Strain Release and Defect Passivation in Formamidinium-Dominated Perovskite via a Novel in-Plane Thermal Gradient Assisted Crystallization Strategy.

It is essential to release annealing induced strain during the crystallization process to realize efficient and stable perovskite solar cells (PSCs), which does not seem achievable using the conventional annealing process. Here we report a novel and facile thermal gradient assisted crystallization strategy by simply introducing a slant angle between the preheated hot plate and the substrate. A distinct crystallization sequence resulted along the in-plane direction pointing from the hot side to the cool side, which effectively reduced the crystallization rate, controlled the perovskite grain growth, and released the in-plane tensile strain. Moreover, this strategy enabled uniform strain distribution in the vertical direction and assisted in reducing the defects and aligning the energy bands. The corresponding device demonstrated champion power conversion efficiencies (PCEs) of 23.70% and 21.04% on the rigid and flexible substrates, respectively. These highly stable rigid devices retained 97% of the initial PCE after 1097 h of storage and more than 80% of the initial PCE after 1000 h of continuous operation at the maximum power point. This novel strategy opens a simple and effective avenue to improve the quality of perovskite films and photovoltaic devices via strain modulation and defect passivation.