钙钛矿是一种新型的半导体材料，在太阳能电池、发光二极管器件、光电探测等领域具有广泛的应用前景。通过控制钙钛矿材料在溶液中的结晶过程，能够提升钙钛矿材料的质量，并进一步提升钙钛矿器件的性能。钙钛矿的结晶过程一般采用溶剂工程、添加剂工程和界面工程等方法调控，然而这些方法是基于给定条件下的自发过程，缺少时空控制能力，限制了钙钛矿材料质量的提升。本论文提出了光微流诱导结晶机理，利用飞秒激光在时空上调控钙钛矿的结晶过程，阐述了激光-配体协同调控作用，开发了适用于多种钙钛矿材料的飞秒激光诱导单晶生长技术。基于该技术实现了高质量钙钛矿单晶微图案和薄膜的制备。提出光微流诱导结晶机理，利用光热效应和气液界面带来的蒸发和对流，高效地构建局域、可控的过饱和度，实现对钙钛矿单晶生长过程的调控。通过COMSOL有限元模拟从理论上证明了光微流诱导结晶机理的正确性，并通过实验验证该机理。基于该机理，可在优化的制备条件下，得到无激光损伤的钙钛矿单晶结构，制备速度可达100 μm/s，所得结构具有良好的光致发光性能。提出激光-配体协同调控策略，以解决钙钛矿结构自发生长引起的形貌不可控的问题。研究不同配体种类和浓度对MAPbBr3钙钛矿生长过程的影响，通过配体条件优化，抑制自发生长，实现形貌可控的制备过程。基于激光-配体协同调控作用开发了飞秒激光诱导钙钛矿单晶生长技术，通过该技术制备了具有光滑表面形貌、良好的荧光性质和低缺陷浓度的钙钛矿单晶复杂图案化结构。通过前驱体、配体以及激光参数的优化，将飞秒激光诱导钙钛矿单晶生长技术拓展至FAPbBr3、MAPbCl3、MAPbI3、CsPbBr3钙钛矿材料中，证明该技术具有普适性。针对激光逐点扫描制备钙钛矿薄膜过程中加工效率低的问题，通过光斑整形和激光-半月板界面协同控制机理设计加工装置，实现了线光斑扫描下钙钛矿单晶薄膜的快速制备。实验结果表明，利用设计的加工装置，能够得到高表面质量，低缺陷浓度的钙钛矿薄膜，最优加工条件下加工效率为0.0216 mm2/s。该方法可以通过使用更长的线光斑并提升扫描速度的方式进一步提升加工效率，具有制备钙钛矿器件的潜力。

Perovskite is an emerging semiconductor material with broad application prospects in solar cells, light-emitting diodes, photodetectors, and other fields. Controlling the crystallization process of perovskite materials contributes to enhance the quality of perovskite materials and further improve the performance of perovskite devices. Traditionally, the crystallization process of perovskites is regulated through solvent engineering, additive engineering, and interfacial engineering. However, these methods are based on spontaneous processes under given conditions and lack spatiotemporal control capabilities, which limits the enhancement of perovskite material quality. This study proposes a laser-induced crystallization mechanism named as optofluidic crystallithography, and utilizes femtosecond laser to spatiotemporally control the crystallization process of perovskites. The synergistic control mechanism of laser and ligands is elaborated. A femtosecond laser-induced single-crystal growth technique is developed which is applicable to various perovskite materials. Based on this technique, high-quality perovskite single-crystal micropatterns and thin films have been successfully fabricated.The optofluidic crystallithography was proposed, which can efficiently create localized, controllable supersaturation by leveraging the photothermal effect and the evaporation and convection at the gas-liquid interface, and achieve control over the growth process of perovskite single crystals. The correctness of the optofluidic crystallithography mechanism was proved theoretically by COMSOL finite element simulation, and was verified by experiment. Based on this mechanism, the single crystal structure of perovskite without laser damage can be obtained under optimized preparation conditions. The preparation speed can reach 100 μm/s. The obtained structure has good photoluminescence performance.The problem of uncontrollable morphology caused by spontaneous growth of perovskite structure was solved by using laser-ligand co-regulation. The study investigated the effects of different ligand types and concentrations on the growth process of MAPbBr3 perovskite. By optimizing ligand conditions, spontaneous growth was inhibited and the morphology controllable preparation process was realized. A femtosecond laser-induced perovskite single crystal growth technique was developed based on the laser-ligand co-regulation. By this technique, the complex pattern structures of perovskite single crystal with smooth surface morphology, good fluorescence properties and low defect density were prepared. By optimizing the precursor solution, ligand conditions, and laser fabrication conditions, the femtosecond laser-induced perovskite single crystal growth technique was extended to FAPbBr3, MAPbCl3, MAPbI3, CsPbBr3 perovskites, proving the universality of the technique.To address the issue of the low processing efficiency in preparation of perovskite thin film by laser point-by-point scanning, a processing device was designed based on beam shaping and the synergistic control mechanism of laser and meniscus interface, which enabled rapid preparation of perovskite single-crystalline thin films under line spot scanning. It was indicated that the designed processing device can prepare perovskite thin films with high surface quality and low defect density. The optimal processing conditions yield a processing efficiency of 0.0216 mm2/s. This processing efficiency of this method can be further improved by using a longer line spot and improving the scanning speed, which is potential to prepare perovskite devices.