C-Photo: Computational photochemistry and in silico design of MOST systems

C-Photo：计算光化学和 MOST 系统的计算机设计

• 批准号: 517844450
• 负责人: Professor Dr. Andreas Dreuw
• 金额: --
• 依托单位: Chair of Theoretical and Computational Chemistry
• 依托单位国家: 德国
• 项目类别: Research Units
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/517844450?language=en
• 关键词: Photo; Computational; photochemistry; silico; design

The utilization of solar energy is the most promising pathway to cover the energy demands of our modern society. A largely unexplored concept is in this context the molecular solar thermal (MOST) energy conversion process, which releases heat through photochemically triggered chemical transformations on demand. In the proposed research unit FOR MOST, this concept is to be explored from a fundamental research point of view in concert of synthesis, spectroscopy, theory and application. This proposal covers the theoretical part with emphasis on the photochemical and spectroscopical aspects. In detail, genetic algorithms and machine learning approaches will be used to explore the vast chemical space of different MOST systems by pre-screening for the most promising MOST molecules, so-called mostophores. Further detailed quantum chemical investigations using our self-developed excited-state methods but also all other available theoretical tools complement the efforts. The “best” candidates will then be synthesized and spectroscopically investigated with focus on optimal MOST properties, for example, a high energy-to-mass ratio, favorable overlap with the solar spectrum and appropriate storage times together with the other FOR MOST partners. Within this project, we will investigate in detail the photochemical switching mechanisms into the storage state of coupled azobenzenes, azaborines and norbornadiene as well as of hybrid systems. We will thereby help to design novel mostophores by a priori in silico design, by straightforward derivatization as well as by exploitation of molecular interactions for the stabilization of the storage state. A further important contribution of this project is the simulation of optical spectra of the mostophores in their molecular environments to guide the interpretation of static and time-resolved experimental spectra using our self-developed quantum chemical methodology and environment models. Along the same lines, we will investigate the possibility of oxidative and/or reductive switching of the mostophores, i.e. by electron detachment and attachment. The switching mechanisms will be computed and electronic spectra of the intermediates will be simulated to guide experimental investigations. The theoretical efforts undertaken in this project are thus well embedded into the FOR MOST research unit and will contribute substantially the collaborative projects.

太阳能的利用是涵盖我们现代社会能源需求的最有希望的途径。一个很大的意外概念是在这种情况下，分子太阳能热（大多数）能量转换过程，该过程通过按需光化学触发的化学转化来释放热量。在大多数人提出的研究单位中，该概念应从合成，光谱，理论和应用的基本研究的观点探讨。该建议涵盖了理论部分，重点是光化学和光谱方面的方面。详细说明，遗传算法和机器学习方法将用于通过预筛查最有希望的大多数分子，即所谓的大多数人，探索大多数系统的庞大化学空间。进一步详细的量子化学投资，使用我们的自发兴奋状态方法，以及所有其他可用的理论工具完成工作。然后，将合成“最佳”候选人，并在光谱镜上研究和侧重于最佳大多数特性，例如，高能量与质量比，与太阳能光谱和适当的存储时间有利的重叠以及大多数合作伙伴的适当存储时间。在该项目中，我们将详细研究光化学切换机制，以耦合的叠氮苯甲苯，阿扎邦和北苯二烯以及混合系统的储存状态。因此，我们将通过直接的衍生化以及通过剥削分子相互作用来帮助设计新颖的Moverphores，以稳定储存状态。该项目的另一个重要贡献是模拟了Mostphores在其分子环境中的光谱，以指导使用我们的自开发的量子化学方法和环境模型来指导静态和时间分辨实验光谱的解释。按照相同的线路，我们将研究大多数载体的氧化和/或减少开关的可能性，即通过电子脱离和附着。将计算开关机制，并将模拟中间体的电子光谱以指导实验投资。因此，该项目所做的理论努力已被很好地嵌入到大多数研究部门中，并将为协作项目做出重大贡献。