Optical (micro)spectroscopy for characterizing structure and electronic properties of self-healing materials for energy conversion and storage

该项目将通过多模态频率和时间分辨光谱学表征能量转换和存储的自修复材料的分子机制。这些实验将提供对功能性自愈材料从损伤到愈合的完整生命周期的见解。在此过程中，该项目将详细了解聚合物基电池和超级电容器以及有机太阳能电池功能材料愈合过程中发生的分子过程。为此，该项目的重点有三个方面：(i)通过原位振动光谱和振动光谱电化学结合二维相关分析，研究降解和自修复过程中的分子结构变化，以获得与潜在可逆自修复化学相关的结构-性质关系；（ii）通过结合荧光和非线性拉曼显微镜，研究运输和化学反应性，为FuncHeal研究的自修复功能材料的扩散和自修复过程提供分子观点。在这里，分子观点将与宏观愈合研究相关联，从而能够调整材料内部的分子成分，以实现所需的宏观性能；（iii）表征受损和愈合材料中的激发态过程，以进行能量转换，以验证聚合物太阳能电池自愈材料中的光诱导功能决定过程。此外，该项目致力于利用光激发聚合物材料的光谱特征来生成指标，以跟踪材料降解和愈合的动力学。

The project will characterize the molecular mechanism in self-healing materials for energy conversion and storage by means of multimodal frequency- and time-resolved optical spectroscopy. The experiments will provide insights into the complete lifecycle of a functional self-healing material from damage to healing. In doing so, the project will gain a detailed understanding of the molecular processes occurring during healing of functional materials For polymer-based batteries and supercapacitors as well as organic solar cells. To this end, the project’s focus is threefold: (i) Investigation of the molecular structure changes during degradation and self-healing via in-situ vibrational spectroscopy and vibrational spectroelectrochemistry in combination with 2D correlation analysis to derive structure-property relationships with respect to the underlying reversible self-healing chemistry; (ii) Studying transport and chemical reactivity to provide a molecular view on the diffusion and thus self-healing processes of the self-healing functional materials researched within FuncHeal, by combining fluorescence and non-linear Raman microscopy. Here, the molecular view will be correlated with macroscopic healing studies to enable tuning the molecular components inside the materials to achieve the desired macroscopic properties and (iii) characterizing excited-state processes in damaged and healed materials for energy conversion to validate the light-induced function-determining process in self-healing materials for polymer solar cells. Furthermore, the project strives towards utilizing the spectroscopic signature of optically excited polymer materials to generate metrics to follow the kinetics of material degradation and healing.