Effects of Proton Beam and Solar Light Irradiation in Multiple-cation Halide Perovskites

卤化物钙钛矿，包括杂化无机有机钙钛矿（HIOPs）已经彻底改变了光电子学领域，因为它们有前途的器件相关特性，包括高吸收系数，高载流子迁移率和低激子结合能值，与光伏，发光二极管和光电探测器相关。近年来，钙钛矿薄膜的器件应用已经得到了广泛的研究，但对温度、湿度和高能辐射等外部刺激因素的影响仍未得到明确的认识。由于内在和外在效应都会影响钙钛矿材料的光物理性质，因此详细了解外部刺激（如辐射效应）对于进一步优化太阳能电池器件至关重要。这个德法联合研究小组将研究通过质子（H+）辐照增加钙钛矿材料的缺陷容忍度，从而提高钙钛矿材料稳定性的基本方面。H+BOOST项目的科学目标是针对复合工程的多阳离子HOIPs，这些HOIPs将通过高能质子辐照处理硬化到原子级缺陷。该研究的中心目标是证明钙钛矿太阳能电池在~1 MeV质子辐照下的合成后处理是否可以应用于不同的HOIPs光伏器件结构，并适应其他HOIPs组成，以提高其环境和操作稳定性。此外，我们将系统地研究通过~1 MeV质子辐照诱导的四阳离子铅钙钛矿的内在点缺陷的作用，以阐明缺陷辅助过程与PV在老化过程中的稳定性和耐久性有关。该项目结合了德国研究小组在化学工程方面的专业知识，包括定义的HIOP单晶和薄膜，以及它们在太阳能电池设备中的集成，以及法国合作伙伴在质子辐照和空间分辨显微镜和光谱学方面的专业知识，以将缺陷形成与太阳能电池性能联系起来。

Halide perovskites including hybrid inorganic organic perovskites (HIOPs) have revolutionized the field of optoelectronics due to their promising device-related properties that include high absorption coefficients, high charge-carrier mobilities and low exciton binding energy values relevant for photovoltaics, light-emitting diodes, and photodetectors. While the device applications of perovskite thin films have been extensively investigated in the recent years, unambiguous understanding on the influence of external stimulants such as temperature, humidity and high-energy radiation remains elusive. Since both intrinsic and extrinsic effects can influence the photo-physical properties of perovskite materials, detailed understanding of external stimuli such as radiation effects is crucial for further optimization of solar cell devices. This German-French consortium will investigate fundamental aspects of improving the stability of perovskite materials by increasing their defect-tolerance through proton (H+) irradiation. The scientific objectives of the H+BOOST project will target compositionally engineered multiple-cation HOIPs that will be hardened towards atomic level defects by high-energy proton irradiation treatments. The central goal is to demonstrate whether a post-synthesis processing of perovskite solar cells with ~1 MeV proton irradiation can be applied to different HOIPs PV device architectures and adapted to other HOIPs composition for enhancing their environmental and operational stability. Moreover, the compositionally engineered quadruple-cation lead perovskites will be systematically investigated towards the role of intrinsic point defects induced via ~1 MeV proton irradiation to clarify defect-assisted processes relevant to PV stability and durability during ageing. This project combines the complimentary expertise of the German research group in chemical engineering of defined HIOP single crystals and thin films as well as their integration in solar cell devices with the expertise of the French partners in proton irradiation and spatially resolved microscopy and spectroscopy to correlate defect formation with solar cell performance.