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Excimer Formation in Carboxylic Acid-Functionalized Perylene Diimides Attached to Silicon Dioxide Nanoparticles
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2019-02-05 , DOI: 10.1021/acs.jpcc.8b12061
Jeffrey Gorman 1 , Raj Pandya 1 , Jesse R Allardice 1 , Michael B Price 2 , Timothy W Schmidt 3 , Richard H Friend 1 , Akshay Rao 1 , Nathaniel J L K Davis 2
Affiliation  

The creation of artificial light-harvesting complexes involves the ordered arrangement of chromophores in space. To guarantee efficient energy-transfer processes, organic dyes must be brought into close proximity, often leading to aggregation and the formation of excimer states. In recent years, the attachment of ligand-based chromophores to nanoparticles has also generated interest in relation to improved solar harvesting and spin-dependent electronic interactions such as singlet fission and upconversion. We explore the covalent attachment of two novel perylene-diimide (PDI) carboxylic acid ligands to silicon dioxide nanoparticles. This allows us to study electronic interactions between the ligands when attached to nanoparticles because these cannot couple to the wide band gap silicon dioxide. One of the synthesized PDI ligands has sterically hindering phenols in the bay position and undergoes minimal optical changes upon attachment, but the other forms an excimer state with a red-shifted and long-lived florescence. As such, molecular structure changes offer a method to tune weak and strong interactions between ligand layers on nanocrystal surfaces.

中文翻译:

附着在二氧化硅纳米颗粒上的羧酸官能化苝二酰亚胺中准分子的形成

人工光捕获复合体的创建涉及发色团在空间中的有序排列。为了保证有效的能量转移过程,有机染料必须非常接近,这通常会导致聚集并形成准分子态。近年来,基于配体的发色团与纳米颗粒的附着也引起了人们对改善太阳能收集和自旋依赖性电子相互作用(例如单线裂变和上转换)的兴趣。我们探索了两种新型苝二酰亚胺(PDI)羧酸配体与二氧化硅纳米粒子的共价连接。这使我们能够研究连接到纳米颗粒上的配体之间的电子相互作用,因为它们不能与宽带隙二氧化硅耦合。合成的 PDI 配体之一在海湾位置具有空间位阻酚,并且在连接时经历最小的光学变化,但另一种形成具有红移和长寿命花期的准分子态。因此,分子结构的变化提供了一种调节纳米晶体表面配体层之间弱相互作用和强相互作用的方法。
更新日期:2019-02-06
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