Functionalized cage hydrocarbons and their applications as white light emitters

该项目的重点是制备有机白光产生(WLG)材料，其基础是钻石状和立方体核心，这些核心配备了改变决定发射特性的分子性质的功能。这包括对WLG的合适候选者进行预筛选，然后将在For 2824的其他组中测量其团簇形态以及物理性质。我们还将利用密度泛函理论进行初步的计算筛选，以评估官能团取代的效果。四个一般性的基本问题将被解决：1)高度对称的分子核心结构的WLG的反转对称性起什么作用？这将用金刚烷(D3d)和立方烷(OH)核进行探测，并与已建立的金刚烷(TD)衍生物进行比较。2)玻璃是否是诱导WLG的最佳和可复制的非晶态物质？3)在类似的脉络中，聚合物是否适合WLG材料？4)合成方法和随后的材料在供应链、成本、易于处理、降解和重复使用方面是否可持续？这将通过四个工作包(WP)来解决：WP1)描述了新的核心材料的合成及其性能的微调：由于金刚烷核心已被证明是一种有价值的WLG构建块，我们将把我们的研究扩展到类似的金刚烷和相关的具有各种取代基的立方烷衍生物(具有电子给体和受体取代的取代芳基体系)。WP2)考察了互补的有机和无机(来自A1(Dehnen))材料的无定形性的影响和控制。随着最近成功地通过与A1(Dehnen)的材料混合来重复制备我们的材料和共晶混合物的玻璃，我们的目标是探索这种物质状态，因为它是一种更简单的生产非晶态材料的方法。其次，玻璃涂层很容易适应各种应用，我们将确定在哪些表面上可以制备玻璃，从玻璃上的玻璃开始，直接利用WLG。WP3)涉及可生物降解聚合物的制备和测试，作为获得也可持续的无定形材料的替代品。聚合物将为应用提供许多机会，例如用于需要柔韧性的WLG涂料。从一开始，我们将只使用聚酯和聚酰胺键来实现生物降解性。WP4)支持对所提议的单分子结构的分子性质进行计算预筛选以指导合成的实验研究。

The project focuses on the preparation of organic white-light generating (WLG) materials based on diamondoid and cubane cores that are equipped with functionality to alter the molecular properties that determine the emission characteristics. This includes pre-screening of suitable candidates for WLG, whose cluster morphologies as well as physical properties will then be measured in other groups of FOR 2824. We will also undertake preliminary computational screens utilizing density functional theory to evaluate the effects of functional group substitution. Four general fundamental questions will be addressed: 1) What is the role of inversion symmetry for WLG of the highly symmetric molecular core structure? This will be probed with diamantane (D3d) and cubane (Oh) cores and compared to the established adamantane (Td) derivatives. 2) Are glasses optimal and reproducible amorphous states of matter to induce WLG? 3) In a similar vein, are polymers suitable WLG materials? 4) Are the synthetic approaches and the ensuing materials sustainable with respect to supply chain, cost, ease of handling, degradation, and re-use? This will be tackled in four work packages (WP): WP1) describes the synthesis of new core materials and fine-tuning of their properties: as the adamantane core has proven to be a valuable WLG building block, we will expand our studies to analogous diamantane and related cubane derivatives with a variety of substituents (substituted aryl systems with electron donor and acceptor substitution). WP2) examines the influence and control of amorphousness of complementary organic and inorganic (from A1 (Dehnen)) materials. With the recent success in reproducibly preparing glasses of our materials and eutectic mixtures through blending with materials from A1 (Dehnen), we aim at exploring this state of matter because it is a much simpler way to produce amorphous materials. Secondly, glass coatings are readily amenable to a variety of applications, and we will determine on which surfaces glasses can be prepared, starting with glass-on-glass to exploit WLG directly. WP3) concerns the preparation and testing of biodegradable polymers as alternatives to access amorphous materials that can also be made sustainable. Polymers would offer many opportunities for applications such as for coatings for WLG where flexibility is needed. From the start, we will implement biodegradability by using polyester and polyamide linkages only. WP4) supports the experimental studies computational pre-screening of molecular properties of proposed single-molecule structures to guide synthesis.