宽带隙钙钛矿材料的筛选数据

该子数据集包括依据计算机模拟研究下的带隙位于1.65-1.75eV之间的钙钛矿材料的优选方案，设计替换与混合A位阳离子、金属或卤素原子，并分析其与带隙的构效关系；其中，A位基团最外层p电子轨道与铅最外层s轨道间相互作用的强弱，可调节ABX3材料的带隙，基于此，合理设计出了不同比例的小尺寸和中等尺寸A位离子掺杂的结构体系；B位阳离子的类型改变会对晶体结构造成维度上的影响，往往倾向于向低维结构发展，进而造成带隙的改变，基于该理论指导，成功设计制备出了MA3Sb2I9−xClx系列结构，且得到了与理论指导相符合的带隙变化规律；卤素离子的掺杂是调节带隙的常用手段，对X位基团进行了卤素和拟卤素的掺杂和取代，并系统地分析其对稳定性和带隙的影响规律，结果证明，X位掺杂拟卤素后可以增加材料的稳定性，禁带宽度随掺杂OCN- 、SCN-、SeCN-、TeCN-的顺序降低；X位掺杂离子半径较小的卤素离子会增加晶体的禁带宽度，增加晶体的结构稳定性，由此预测了带隙在1.65-1.75eV范围内的宽带隙钙钛矿组分比例，并通过实验进一步细化了A位的微量掺杂组分，获得了3种稳定的混合卤素宽带隙钙钛矿组分。晶体结构不同位置的掺杂与离子尺寸的变化与带隙构效关系的确定为之后的器件性能的提升提供一定的理论指导。

This sub-dataset contains optimized perovskite material candidates with band gaps between 1.65 and 1.75 eV, developed based on computational simulation studies. We designed substitutions and mixed modifications of A-site cations, metal or halogen atoms, and systematically analyzed the structure-band gap relationships of these modifications. Specifically, the strength of the interaction between the outermost p orbital electrons of the A-site group and the outermost s orbital electrons of lead can modulate the band gap of ABX3-type perovskite materials. Leveraging this mechanism, we rationally designed structural systems doped with small-sized and medium-sized A-site ions at varying doping ratios. Changes in the type of B-site cations induce dimensional modifications to the crystal structure, which typically tend to evolve toward low-dimensional architectures, thereby altering the band gap. Guided by this theoretical framework, we successfully designed and synthesized the MA3Sb2I9−xClx series of structures, and obtained band gap variation trends consistent with the theoretical predictions. Halide ion doping is a widely used strategy for modulating band gaps. We performed doping and substitution of both halogens and pseudohalogens on the X-site groups, and systematically analyzed their effects on material stability and band gap variation trends. The results show that doping the X-site with pseudohalogens can improve material stability, and the band gap decreases in the order of OCN⁻, SCN⁻, SeCN⁻, and TeCN⁻ doping. Doping the X-site with halide ions of smaller ionic radii can increase the crystal's band gap and enhance its structural stability. Based on these findings, we predicted the composition ratios of wide-band-gap perovskites with band gaps ranging from 1.65 to 1.75 eV, and further refined the trace doping components of the A-site via experiments, ultimately obtaining three stable mixed-halide wide-band-gap perovskite compositions. The establishment of the structure-band gap relationships involving doping at various positions of the crystal structure and variations in ionic radii provides valuable theoretical guidance for subsequent improvements in device performance.

搜集汇总

背景与挑战

背景概述

该数据集包含宽带隙钙钛矿材料的筛选数据，通过计算机模拟研究，优选了带隙位于1.65-1.75eV之间的钙钛矿材料，并分析了A位、B位和X位掺杂对带隙的影响规律。数据集提供了3种稳定的混合卤素宽带隙钙钛矿组分，为器件性能提升提供了理论指导。