Modular artificial photosystems based on polymers

该研究计划致力于创建人工分子光系统，并探索其在能量转换方案中的潜力。为了实现这一目标，将采用模块化工具箱方法，该方法以前证明大大减少了综合工作。所需的功能是基于通过定制的构建块断开基本步骤（能量和电子转移）-这使得基于聚合物的架构的指导开发成为可能。许多可能的结构的选择和选择源于固有的光学和电化学性质，它们将在适当的时候结合起来。光诱导电荷分离是至关重要的，尽管组装策略可以适应其他应用领域的需要。在第一个工作包中，将合成分子结构不同的组成构件。此外，可聚合基团以及增溶基团将被引入，这是在下面的包中所需要的。在第二个工作包中，分子结构将通过电化学活性结构单元的聚合来组装。所获得的电子和空穴传输聚合物将在最后两个步骤中连接到染料单元。值得注意的是，确保了物质库的简易模块化合成，这在遵循经典方法的相关分子组装体的情况下在合成上是非常苛刻的。在第三个工作包中，将使用时间分辨光谱来探索光致电荷分离及其复合。因此，将探索各种分子参数（例如链长、共轭类型、内部电荷级联），以使重组最小化。该研究从溶液中的研究开始，通过薄膜形成到固态，以评估下降项目和建议的潜力。该研究项目的目的和好处是建立一个分子水平的模块化平台，以在纳米级水平上创建和控制电荷和激发态。这种控制与能量转换的许多应用相关，例如耦合催化反应、分子运动或产生外部电化学势。值得注意的是，模块化特征允许以直接的方式用更合适的组件替换单个组件，这对于其他分子结构的设计也是理想的，并为其他应用和进一步的下行项目奠定了基础。

This research proposal is dedicated to create artificial molecular photosystems and to explore their potential in energy conversion schemes. In order to reach this goal, a modular toolbox-approach will be followed, which previously testified a significantly reduced synthetic effort. The desired function is based on the disconnection of elementary steps (energy- and electron transfer) by tailored building blocks – which enable the guided development of polymer-based architectures. The choice and selection of the many conceivable structures originates from the inherent optical and electrochemical properties, which are to be combined in due course. The light-induced charge separation is of key importance albeit the assembly strategy can be adapted to the needs of other fields of applications. In the first work package, the constitutional building blocks will be synthesized, which differ in their molecular structure. Moreover, polymerizable groups as well as solubility-promoting groups will be introduced, which are required in the following packages.In the second work package, molecular architectures are to be assembled via polymerization of electrochemically active building blocks. The obtained electron- and hole-transporting polymers will be attached t in the final two steps to a dye unit. Noteworthily, the facile modular synthesis of substance libraries is ensured, which is synthetically very demanding in case of related molecular assemblies following a classical approach. In the third work package, the light-induced charge separation and recombination thereof is to be explored using time-resolved spectroscopy. Hence various molecular parameters will be explored (e.g. chain length, kind of conjugation, internal charge cascades), in order to minimize the recombination. The studies embark from investigation in solution towards the solid state via film formation, in order to evaluate the potential for descending projects and proposals.The aim and benefit of this research project is to establish a modular platform on a molecular level, in order to create and to control electric charges and excited states on a nanoscopic level. Such control is relevant for many applications of energy conversion, e.g. coupled catalytic reactions, molecular motion, or to generate an external electrochemical potential. Noteworthily, the modular character permits the replacement of individual components by better-suited ones in a straight forward fashion, which is desirable also for the design of other molecular architectures and founds the basis for other applications and further descending projects.