Hybrid organic-inorganic perovskites (HIOPs) have increasingly promoted the photovoltaic field due to their excellent semiconductor properties and inexpensive costs. Interdiffusion protocol has been regarded as an efficient approach to deposit high-quality HIOP films. Nevertheless, the underlying mechanism of this protocol remains obscured. In this work, in virtue of vapor-deposited lead halide frame to eliminate solution-driven lead halide effect, we thoroughly studied the evolution of different HIOP films by symmetrically controlling the initial lead halides as well as organic salts. The crystal growth mechanism of the interdiffusion can be drawn in two aspects: 1. CH₃NH₃ (MA)-HIOP shows higher nucleation rate than (NH₂)₂CH (FA)-HIOP; 2. FA-HIOP and PbCl₂-HIOP exhibit greater coarsening rates than other colleagues. Most importantly, conflicting lattice with Cl-barren phase and Cl-rich phase is first uncovered for MA-HIOP and FA-HIOP using PbCl₂ frame. All the device performances based on these films also prove the potential mechanism, and champion efficiency of 16.01% is achieved based on FAPbI₃. This work will provide in-depth insight into the interdiffusion protocol and drive this protocol toward multiple photovoltaic applications by facilely controlling precursor compositions.

杂化有机-无机钙钛矿（HIOPs）由于其优异的半导体性能和廉价的成本而日益促进了光伏领域。互扩散协议已被视为沉积高质量HIOP薄膜的有效方法。但是，该协议的基本机制仍然被掩盖。在这项工作中，借助气相沉积的卤化铅框架消除溶液驱动的卤化铅效应，我们通过对称地控制初始卤化铅以及有机盐彻底研究了不同HIOP膜的演变。互扩散的晶体生长机理可以从两个方面得出：1. CH ₃ NH ₃（MA）-HIOP的成核速率高于（NH ₂）_2。CH（FA）-HIOP; 2. FA-HIOP和PbCl ₂ -HIOP的粗化率高于其他同事。最重要的是，首先使用PbCl ₂框架发现了MA-HIOP和FA-HIOP与Cl贫瘠相和富Cl相冲突的晶格。基于这些薄膜的所有器件性能也证明了潜在的机理，基于FAPbI ₃达到了16.01％的冠军效率。这项工作将提供对互扩散协议的深入了解，并通过方便地控制前驱体成分将协议推向多种光伏应用。