Multidimensional photoresponsive molecular architectures for high performance solar cells

本项目旨在了解、开发和应用基于低带隙分子组装成多维结构的光电功能，以实现下一代高性能体异质结（BHJ）有机太阳能电池（OSCs）。我们的整体方法包括新的供体(D)和受体(A)的分子网络，光增强电荷传输结合形态控制和创新的光增强或收获结构。虽然先前研究的关键OSC参数如能级匹配和载流子迁移率可以在制造前筛选，但优化的核心活性层形态很难通过简单的分子结构分析来预测。在即将到来的项目中，我们将利用我们之前的研究结果，结合基于自组装网络和光诱导有源层结构的改进构建块，从形态学分析到系统形态学和体系结构控制进行范式转变。对于内部OSC结构，我们将合成创新的苝酰亚胺A衍生物，这些衍生物的官能团经过优化，可以实现复杂的二维和三维结构。通过将材料设计、合成和光伏评价有效地结合起来，我们将利用我们最初的增强D- a材料的类醌共振的概念，识别出高迁移率、低带隙的D材料。协同A和D优化将导致高性能的非富勒烯osc。虽然这一途径将在纳米尺度上影响分子秩序，但光辅助过程，如通过交联或光诱导传质进行的光图图化，将在微尺度上与D和A的发展和理论建模不断相互作用，构建活性层。图图化不仅可以用于增强电荷的分离和转移，还可以用于生成外部导光和重分布的光子结构，例如基于结构光聚合物的非周期结构或表面浮雕光栅，从而大大提高整体性能。因此，我们使用光作为形态和表面结构和光收集的控制单元。多尺度建模将提供对D和a组分的分子结构和电子性质与OSC效率之间关系的基本理解。结合量子力学计算与原子和粗粒度分子动力学，我们将预测自组装或光模式网络的形状，支持先进形态的发展。研究了分子迁移率和堆叠以及聚合物纠缠或有序/无序转变对整体电子性能的影响。因此，理论将有助于建立进一步优化盐含量的设计规则。

This project aims to understand, develop, and apply optoelectronic functionalities based on the assembly of low band gap molecules into multidimensional architectures for the realization of next generation high-performance bulk heterojunction (BHJ) organic solar cells (OSCs). Our integral approach includes molecular networks of novel donors (D) and acceptors (A), photoenhanced charge transport combined with morphology control and innovative light enhancing or harvesting structures. While crucial OSC parameters as energy level matching and charge carrier mobility, studied previously, can be screened prior to fabrication, active layer morphology, which is central for optimization, is hard to predict by simple molecular structure analysis. In the upcoming project, we will exploit our previous results to perform a paradigm shift from morphology analysis to systematic morphology and architecture control combined with improved building blocks based on self-assembled networks and light-induced active layer structuring.For the inner OSC structure, we will synthesize innovative perylene bisimide A derivatives that are optimized in their functional groups allowing complex 2d and 3d structures. By effectively combining material design, synthesis, and photovoltaic evaluation, we will identify high-mobility, low-bandgap D materials, employing our original concept of enhancing the quinoid resonance of D-A materials. Synergetic A and D optimization will lead to high-performance non-fullerene OSCs.While this route will influence molecular order on the nanoscale, light-assisted processes like photo-patterning via crosslinking or photo-induced mass transfer will structure the active layer on the microscale, in constant interplay with D and A development and theoretical modeling. Patterning will not only be used to enhance charge separation and transfer, but also to generate outer light-guiding and redistributing photonic structures, e.g. aperiodic structures or surface relief gratings based on structured photopolymers, considerably improving the overall performance. Thus, we employ light as a control unit for both morphology and surface structuring and light harvesting.Multiscale modeling will provide a fundamental understanding of the relation between molecular structure and electronic properties of the D and A components and the OSC efficiency. Combining quantum-mechanical calculations with atomistic and coarse-grained molecular dynamics, we will predict the shape of self-assembled or photo-patterned networks, supporting the development of an advanced morphology. The effect of molecular mobility and stacking as well as polymer entanglement or order/disorder transitions on the overall electronic properties is studied. Thus, theory will contribute to establishing design rules for further OSC optimization.