volatile decomposition [23] or halide segregation are often observed in hybrid perovskites under various stress conditions (light, [24] thermal, [25] and electric fields [26]); 4) spontaneous phase transition easily occurs for perovskite with unstable crystal structures, particularly for inorganic perovskite. [27-29] To improve the stability of PSCs, researchers attempted numerous methods such as encapsulation, [30] additive engineering, [31] component engineering, [32] etc. [33] However, the PSCs' stability is yet to achieve a perfect solution. Recently, researchers found that the introduction of long-chain organic cations in 3D perovskite as 2D perovskite can block water and oxygen molecules, meanwhile, generate a steric effect to prevent phase transitions, and limit ion migration. [34-36] Hence, fabricating 2D [37,38] or 2D/3D [39-43] mixed perovskite as absorbing layers are effective approaches to improve the stability of PSCs. However, the PCE of 2D PSCs remain lower than that of the 3D ones, which is mainly attributed to the introduction of organic macromolecules that blocks the effective extraction and transport of carriers. [44,45] Fortunately, 2D perovskite usually has three arrangements, namely parallel, perpendicular to the glass substrate or randomly arranged. [46] Manipulating the orientation of the crystal and the phase distribution in the 2D solution-processed perovskite can improve the efficiency and reproducibility of the device. Among them, the most desired arrangement for PSCs is the one that perpendicular to the substrate. Therefore, studying the crystallization kinetics of 2D perovskite is curial to effectively control the film forming process and adjust the crystal orientation (perpendicular to the substrate), which can effectively avoid or reduce the adverse effects of the organic molecular layer and improve device efficiency. [47,48] Nevertheless, few review articles were published on this subject. In this review, we mainly focus on the key issue for controlling crystallization kinetics and summarizing the research progress of their effects on various types of 2D PSCs. We also discuss the crystal/natural quantum well (QW) structure and the original stability for 2D PSCs in detail. Finally, remaining challenges and outlooks are presented. 2. Crystal and Natural Quantum Well Structure The material structure has a substantial impact on performance. [49-51] Properties of 2D and 3D perovskites differ 2D perovskites demonstrate higher moisture stability, oxygen content, thermal stability, and a significantly lower ion migration/phase transition occurrence in comparison to 3D perovskite. These advantages imply huge potential for 2D perovskite in commercial applications in the photovoltaic field. However, the horizontal arrangement of the organic layer severely hinders the transport of carriers, and thus, the power conversion efficiency of 2D perovskite solar cells (PSCs) is significantly lower than that of 3D. Controlling the crystallization orientation to achieve rapid carrier transport can effe...

Defects are considered to be one of the most significant factors that compromise the power conversion efficiencies and long‐term stability of perovskite solar cells. Therefore, it is urgent to have a profound understanding of their formation and influence mechanism, so as to take corresponding measures to suppress or even completely eliminate their adverse effects on device performance. Herein, the possible origins of the defects in metal halide perovskite films and their impacts on the device performance are analyzed, and then various methods to reduce defect density are introduced in detail. Starting from the internal and interfacial aspects of the metal halide perovskite films, several ways to improve device performance and long‐term stability including additive engineering, surface passivation, and other physical treatments (annealing engineering), etc., are further elaborated. Finally, the further understanding of defects and the development trend of passivation strategies are prospected.

Introducing hydroiodic acid (HI) as a hydrolysis‐derived precursor of the intermediate compounds has become an increasingly important issue for fabricating high quality and stable CsPbI3 perovskite solar cells (PSCs). However, the materials composition of the intermediate compounds and their effects on the device performance remain unclear. Here, a series of high‐quality intermediate compounds are prepared and it is shown that they consist of DMAI/DMAPbIx. Further characterization of the products show that the main component of this system is still CsPbI3. Most of the dimethylammonium (DMA+) organic component is lost during annealing. Only an ultrasmall amount of DMA+ is doped into the CsPbI3 and its structure is stabilized. Meanwhile, excessive DMA+ forms Lewis acid–base adducts and interactions with Pb2+ on the CsPbI3 surface. This process passivates the CsPbI3 film and decreases the recombination rate. Finally, CsPbI3 film is fabricated with high crystalline, uniform morphology, and excellent stability. Its corresponding PSC exhibits stable property and improved power conversion efficiency (PCE) up to 17.3%.

Metal‐free perovskites (MFPs) with flexible and degradable properties have been adopted in flexible X‐ray detection. For now, figuring out the key factors between structure and device performance are critical to guide the design of MFPs. Herein, MPAZE‐NH4I3 ⋅ H2O was first designed and synthesized with improved structural stability and device performance. Through theoretical calculations, the introducing methyl group benefits modulating tolerance factor, increases dipole moment and strengthens hydrogen bonds. Meanwhile, H2O increases the hydrogen bond formation sites and synergistically realizes the band nature modulation, ionic migration inhibition and structural stiffness optimization. Spectra analysis also proves that the improved electron‐phonon coupling and carrier recombination lifetime contribute to enhanced performance. Finally, a flexible and degradable X‐ray detector was fabricated with the highest sensitivity of 740.8 μC Gyair−1 cm−2 and low detection limit (0.14 nGyair s−1).

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The power conversion efficiency (PCE) of perovskite solar cells (PSCs) has exceeded 25%, showing great potential in the photovoltaic field. However, PSCs often show anomalous current density–voltage (J–V) hysteresis behavior in the forward and reverse scanning directions, which makes it impossible to accurately evaluate the performance of PSCs. Therefore, it is necessary to clearly understand the mechanism of hysteresis and suppress the hysteresis. Herein, the J–V hysteresis behavior in PSCs and strategies to suppress hysteresis is focused: first, the various factors that affect J–V hysteresis in PSCs are summarized. And the mechanism behind the various possible origins of hysteresis and the challenges encountered are explored. Then, the strategies to suppress or eliminate the hysteresis are summarized, including optimizing the perovskite light‐absorbing layer, improving the performance of the carrier transport layer and interface engineering. Finally, insights on the future development of the hysteresis are also provided.

2D perovskite (PEA)2(Cs)n−1PbnI3n+1 (PEA: phenylethylammonium) exhibits more strengthened phase stability than its 3D components under ambient conditions and hence gained great attention in recent years. However, uncontrollable crystallization kinetics in (PEA)2(Cs)n−1PbnI3n+1 leads to difficulty in controlling film morphology and phase‐orientation regulation, resulting in poor power conversion efficiency (PCE). Herein, by incorporating precursor additive N‐methyl‐2‐pyrrolidone iodide (NMPI), the crystallization rate during the deposition of (PEA)2(Cs)n−1PbnI3n+1 film is efficiently regulated. As a result, the 2D or quasi‐2D perovskite solar cell (PSC) delivers record PCEs in all reported 2D or quasi‐2D CsPbX3 families, for instance, the quasi‐2D (n = 20) CsPbI3 PSC exhibits a record PCE of 14.59%, showing significantly enhanced stability. Detailed characterization reveals that the NMPI forms hydrogen bonds with dimethylammonium iodide (DMAI) in the precursor to control crystallization rate for a smooth morphology with small fluctuation, which leads to improved carrier lifetime and reduced trap‐density. More importantly, femtosecond transient absorption (fs‐TA) measurements confirm an improved phase purity and the suppressed nonradiative recombination in quasi‐2D perovskite film. It is believed that this simple additive strategy paves a new route for solving phase transition and crystallization kinetic problems in 2D and quasi‐2D CsPbX3.

Two-dimensional (2D) Ruddlesden-Popper (RP) CsPbI 3 perovskite possesses superior phase stability by introducing steric hindrance. However, due to the quantum and dielectric confinement effect, 2D structures usually exhibit large exciton binding energy, and the charge tunneling barrier across the organic interlayer is difficult to eliminate, resulting in poor charge transport and performance. Here, a multiple-ring aromatic ammonium, 1-naphthylamine (1-NA) spacer is developed for 2D RP CsPbI 3 perovskite solar cell (PSC). Theoretical simulations and experimental characterizations demonstrate that the 2D RP CsPbI 3 perovskite using 1-NA spacer with extended π-conjugation lengths reduces the exciton binding energy and facilitates the efficient separation of excitons. In addition, its cations have a significant contribution to the conduction band, which can reduce the bandgap, promote electronic coupling between organic and inorganic layers, and improve interlayer charge transport. Importantly, the strong π-π conjugation of 1-NA spacer can enhance intermolecular interactions and hydrogen bonding, and prepare high-quality films with preferred vertical orientation, resulting in lower defect density, and directional charge transport. As a result, the (1-NA) 2 (Cs) 3 Pb 4 I 13 PSC exhibits a record 16.62% performance with enhanced stability. This work provides an efficient approach to improve charge transport and device performance by developing multiple-ring aromatic spacers.