Transient-absorption spectroelectrochemistry for studying excited states in electrochemically generated molecular species in solution

瞬态吸收光谱电化学用于研究溶液中电化学生成的分子物质的激发态

• 批准号: 279747293
• 负责人: Professor Dr. Benjamin Dietzek-Ivansic
• 金额: --
• 依托单位: Arbeitsgruppe Molekulare Photonik
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2015
• 资助国家: 德国
• 起止时间: 2014-12-31 至 2019-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/279747293?language=en
• 关键词: Transient; absorption; spectroelectrochemistry; studying; excited

Electron transfer processes are ubiquitous in biology, chemistry and physics. Electron transfer processes present key elementary steps in e.g. photosynthesis and the respiratory chain. Furthermore, (photoinduced) electron transfer steps present the molecular-mechanistic basis for e.g. dye-sensitized solar cells and molecular photocatalysts. During a stepwise electron transfer, irrespective of natural or artificial systems being considered, intermediate reduced/oxidized species are formed, whose photophysics is largely unexploited. The absence of (ultrafast) spectroscopic information about these intermediates is in marked contrast to their functional importance within the electron transfer cascades. Filling this gap in understanding the photoinduced excited-state processes in molecular intermediates of multi-step electron transfer reactions in selected model systems is at the core of this proposal.The project aims at characterizing the photoinduced dynamics in electrochemically produced molecular species in solution by combining cyclovoltammetry and femtosecond time-resolved transient absorption spectroscopy. In doing so the photoinduced processes in exemplarily selected photocatalysts for proton reduction and electron donors for dye-sensitized solar cells in their electrochemically reduced and oxidized forms will be spectroscopically characterized. Hence, the work proposed here will establish a novel approach to study the interplay between structure, dynamics and function of molecular species within an experimental window, which has not been used in previous experiments. Thus, the proposed work will also yield new impulses for further investigations, which will go beyond studying the specific model systems, which are considered here.

电子转移过程在生物学、化学和物理学中普遍存在。电子转移过程是光合作用和呼吸链等过程中的关键基本步骤。此外，（光诱导的）电子转移步骤为例如染料敏化太阳能电池和分子光催化剂提供了分子机理基础。在逐步电子转移过程中，无论考虑天然或人工系统，都会形成中间还原/氧化物种，其物理学基本上未被利用。这些中间体的（超快）光谱信息的情况下，在显着的对比，它们的功能的重要性内的电子转移级联。填补这一空白的理解在选定的模型systems的多步电子转移反应的分子中间体的光诱导激发态过程是在这个proposal.The项目的核心旨在表征光诱导动力学在电化学产生的分子物种在溶液中结合循环伏安法和飞秒时间分辨瞬态吸收光谱。在这样做时，在示例性选择的用于质子还原的光催化剂和用于染料敏化太阳能电池的电子供体中以其电化学还原和氧化形式的光诱导过程将被光谱表征。因此，本文提出的工作将建立一种新的方法来研究结构，动力学和功能的分子物种在实验窗口内，这还没有在以前的实验中使用的相互作用。因此，拟议的工作也将产生新的推动进一步的调查，这将超越研究的具体模型系统，这是考虑在这里。