Conjugated polyelectrolyte-based ternary exciton funnels via liposome scaffolds
Conjugated polyelectrolyte-based ternary exciton funnels via liposome scaffolds
复制标题
通过脂质体支架构建基于共轭聚电解质的三元激子漏斗
DOI：
10.1039/d1me00139f
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发表时间：
2022
影响因子：
3.6
通讯作者：
Ayzner, Alexander L.
中科院分区：
文献类型：
--
作者：
Palmer, Jack;Segura, Carmen J.;Matsushima, Levi;Abrams, Benjamin;Lee, Hsiau-Wei;Ayzner, Alexander L.
人们对开发能够有效地将光子能量转换为化学势能的廉价分子捕光系统有很大的兴趣。非常希望使用自组装并以支持环境友好处理的方式这样做。在任何这样的组件中的关键考虑是吸收太阳能发射光谱的大部分的能力，并且能够有效地将激发态通过空间移动到功能界面。我们以前已经表明，水互共轭双（CPE）复合物可以作为超快和高效的能量转移天线。在这里，我们证明了形成一个分层组装，含水系统的基础上，间CPE激子供体/受体网络和脂质囊泡支架。使用模型小分子有机半导体嵌入在囊泡膜，我们形成一个三元激子漏斗，是面向膜内部。我们发现，虽然能量转移是有效的，组装形态敏感地依赖于制备条件和相对离子化学计量。我们提出了几种方法来稳定这样的水溶液组件。这项工作突出了一个路径形成的水，全色光捕获系统，其功能的复杂性可以系统地增加与模块化。
There is great interest in developing inexpensive, molecular light-harvesting systems capable of efficiently converting photon energy to chemical potential energy. It is highly desirable to do so using self-assembly and in a manner that supports environmentally benign processing. A critical consideration in any such assembly is the ability to absorb a substantial fraction of the solar emission spectrum and to be able to efficiently move excited states through the space to a functional interface. We have previously shown that aqueous inter-conjugated polyelectrolyte (CPE) complexes can act as ultrafast and efficient energy-transfer antennae. Here we demonstrate formation of a hierarchically assembled, aqueous system based on an inter-CPE exciton donor/acceptor network and a lipid vesicle scaffold. Using a model small-molecule organic semiconductor embedded in the vesicle membrane, we form a ternary exciton funnel that is oriented towards the membrane interior. We show that, although energy transfer is efficient, the assembly morphology depends sensitively on preparation conditions and relative ionic stoichiometry. We propose several approaches towards stabilizing such aqueous assemblies. This work highlights a path to formation of an aqueous, panchromatic light-harvesting system, whose functional complexity can be systematically increased with modularity.