Nanoscale phase management of the 2D/3D heterostructure toward efficient perovskite solar cells.

The stabilization of the formamidinium lead iodide (FAPbI3) structure is pivotal for the development of efficient photovoltaic devices. Employing two-dimensional (2D) layers to passivate the three-dimensional (3D) perovskite is essential for maintaining the α-phase of FAPbI3 and enhancing the power conversion efficiency (PCE) of perovskite solar cells (PSCs). However, the role of bulky ligands in the phase management of 2D perovskites, crucial for the stabilization of FAPbI3, has not yet been elucidated. In this study, we synthesized nanoscale 2D perovskite capping crusts with  = 1 and 2 Ruddlesden-Popper (RP) perovskite layers, respectively, which form a type-II 2D/3D heterostructure. This heterostructure stabilizes the α-phase of FAPbI3, and facilitates ultrafast carrier extraction from the 3D perovskite network to transport contact layer. We introduced tri-fluorinated ligands to mitigate defects caused by the halide vacancies and uncoordinated Pb2+ ions, thereby reducing nonradiative carrier recombination and extending carrier lifetime. The films produced were incorporated into PSCs that not only achieved a PCE of 25.39% but also maintained 95% of their initial efficiency after 2000 h of continuous light exposure without encapsulation. These findings underscore the effectiveness of a phase-pure 2D/3D heterostructure-terminated film in inhibiting phase transitions passivating the iodide anion vacancy defects, facilitating the charge carrier extraction, and boosting the performance of optoelectronic devices.

Synergistic Passivation With Phenylpropylammonium Bromide for Efficient Inverted Perovskite Solar Cells.

Inverted perovskite solar cells (PSCs) are a promising technology for commercialization due to their reliable operation and scalable fabrication. However, in inverted PSCs, depositing a high-quality perovskite layer comparable to those realized in normal structures still presents some challenges. Defects at grain boundaries and interfaces between the active layer and carrier extraction layer seriously hinder the power conversion efficiency (PCE) and stability of these cells. In this work, it is shown that synergistic bulk doping and surface treatment of triple-cation mixed-halide perovskites with phenylpropylammonium bromine (PPABr) can improve the efficiency and stability of inverted PSCs. The PPABr ligand is effective in eliminating halide vacancy defects and uncoordinated Pb2+ ions at both grain boundaries and interfaces. In addition, a 2D Ruddlesden-Popper (2D-RP) perovskite capping layer is formed on the surface of 3D perovskite by using PPABr post-treatment. This 2D-RP perovskite capping layer possesses a concentrated phase distribution ≈n = 2. This capping layer not only reduces interfacial non-radiative recombination loss and improves carrier extraction ability but also promotes stability and efficiency. As a result, the inverted PSCs achieve a champion PCE of over 23%, with an open-circuit voltage as high as 1.15 V and a fill factor of over 83%.

Crystallinity and Phase Control in Formamidinium-Based Dion-Jacobson 2D Perovskite via Seed-Induced Growth for Efficient Photovoltaics.

2D perovskites based on Formamidinium (FA) hold the potential for excellent stability and a broad absorption range, making them attractive materials for solar cells. However, FA-based 2D perovskites produced via one-step processing exhibit poor crystallinity and random quasi-quantum wells (QWs), leading to subpar photovoltaic performance. In this study, a seed-induced growth approach is introduced employing MAPbCl3 and BDAPbI4 in the deposition of FA-based Dion-Jacobson 2D perovskite films. This method yields high-quality perovskite films as the seeds preferentially precipitate and serve as templates for the epitaxial growth of FA-based counterparts, effectively suppressing the δ phase. Moreover, the epitaxial growth facilitated by uniformly dispersed seeds results in simultaneous crystallization from top to bottom, efficiently mitigating random phases (n = 2, 3, 4…) induced by the diffusion of organic cations and, in turn, minimizing energy loss. The impact of seed-induced growth on the crystallization and phase distribution of FA-based 2D perovskites is systematically investigated. As a result, the optimized FA-based 2D perovskite solar cell delivers an outstanding efficiency of 20.0%, accompanied by a remarkable fill factor of 0.823. Additionally, the unencapsulated device demonstrates exceptional stability, maintaining 98% of its initial efficiency after 1344 h of storage.