Dion–Jacobson (DJ)‐type quasi‐two‐dimensional perovskites exhibit improved stabilities than their 3D counterparts but meanwhile limited charge transport properties. Knowledge to manipulate the crystal orientation and crystallinity is the primary issue for DJ perovskite with high power conversion efficiencies (PCEs). Herein, the nucleation of DJ perovskite films is divided into three stages and the formation of PbI₂–N,N‐dimethylformamide (DMF)‐based solvated phase (PDS) is highlighted as the initial stage. For the first time, it is demonstrated that regulating the amount of PDS precipitation in stage I by MACl additive is the key to ensure the downward growth of DJ perovskites with out‐of‐plane orientation and high crystallinity in stage III, which is valid for DJ perovskites with different bukly organic cations including p‐phenylenediamine (PPD), p‐xylylenediamine (PXD), and propane‐1,3‐diammonium (PDA). For (PXD)(MA)₂Pb₃I₁₀‐based perovskite solar cells, the PDS engineering lead to a dramtically improved PCE from 1.2% to 15.6%. Moreover, based on temperature‐dependent ionic conductivity measurement, it is confirmed that the ion migration in DJ perovskite films is efficiently suppressed, despite the possible coexisting 3D perovskite phase. The unencapsulated PXD‐based DJ perovskite devices retain over 90% efficiencies after 700 h of continuous illumination or 1500 h of storage in glove box.

中文翻译：

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抑制具有改进的结晶度和垂直方向的Dion–Jacobson钙钛矿的过量溶剂化相

Dion–Jacobson（DJ）型准二维钙钛矿显示出比3D同类更高的稳定性，但同时电荷传输特性有限。具有高功率转换效率（PCE）的DJ钙钛矿的主要问题是控制晶体取向和结晶度的知识。本文将DJ钙钛矿薄膜的成核分为三个阶段，形成PbI ₂ – N，N基于二甲基甲酰胺（DMF）的溶剂化相（PDS）是初始阶段。首次证明，通过MACl添加剂调节第一阶段中PDS沉淀的量是确保第三阶段中具有平面外取向和高结晶度的DJ钙钛矿向下生长的关键，这对DJ钙钛矿具有不同的浅蓝色有机阳离子，包括对苯二胺（PPD），对苯二甲二胺（PXD）和丙烷1,3-二铵（PDA）。对于（PXD）（MA）₂ Pb ₃ I ₁₀PDS工程基于钙钛矿型太阳能电池，可将PCE从1.2％大幅提高至15.6％。此外，基于温度相关的离子电导率测量，可以确认，尽管可能存在3D钙钛矿相，但DJ钙钛矿膜中的离子迁移得到了有效抑制。未封装的基于PXD的DJ钙钛矿设备在连续照明700小时或在手套箱中存储1500小时后仍可保持90％以上的效率。