Electron Transfer in Plexcitonic Systems

我们计划的目的是开发一种新的、模块化的方法来创建光子材料，灵感来自生物光合膜。我们将这种方法称为“分子光子面包板”：最小单元--合成天线复合体--是从零开始设计的，用来在太空中精确地组织分子组件。这些构建块被组装成纳米结构的薄膜。我们将开发激动人心的强光物质耦合新物理，其中激子(分子激发态)与受限光学模式(局域表面等离子体共振)杂交，创建结合光和物质属性的新状态(光激子)。1，2我们的目标是控制从纳米到厘米尺度的能量传递路径，并为分子光子材料设计的革命奠定基础。通过外部扰动控制光过程的能力可能带来操纵光子材料的新方法。在超快时间尺度上，电子和振动自由度之间的耦合(振动耦合)是分子激发态光物理中的关键因素。然而，操纵耦合态是困难的！在本项目中，您将使用强的光-物质耦合到等离子激元模式，以影响和潜在地控制振动耦合，从而控制光驱动反应的结果。这项工作建立在我们之前开发的操纵激发态反应的红外控制方法的基础上。[3]您的项目的一个特别重点将是分子和材料中的电子和能量转移路径，这在光催化和太阳能捕获等应用中可能是重要的。

The aim of our programme is to develop a new, modular approach for the creation of photonic materials, inspired by biological photosynthetic membranes. We call this approach 'molecular photonic breadboards': minimal units - synthetic antenna complexes - are designed from scratch to organise molecular components precisely in space. These building blocks are assembled to form nanostructured films. We will exploit the exciting new physics of strong light-matter coupling, in which excitons (molecular excited states) are hybridised with confined optical modes (localised surface plasmon resonances) to create new states (plexcitons) that combine the properties of light and matter.1,2 Our goal is to control energy transfer pathways from the nm to the cm scale, and is to lay the foundations for a revolution in the design of molecular photonic materials.The ability to control photo-processes by external perturbation could bring a new way to manipulate photonic materials. Coupling between electronic and vibrational degrees of freedom (vibronic coupling) on the ultrafast timescale is the key factor in the photophysics of molecular excited states. However, manipulation of the coupled states is difficult! In this project, you will use strong light-matter coupling to plasmon modes to affect and potentially control vibronic coupling, and hence the outcome of light-driven reactions. This work builds on our previous development of the IR-control approach to manipulate excited state reactions.[3] A particular focus of your project will be on electron and energy transfer pathways in molecules and materials, that might be important in applications including photocatalysis and solar energy capture.