Spin-Exchange and Energy Transfer at Hybrid Molecular/Lanthanide Nanoparticle Interfaces to Control Triplet Excitons

混合分子/稀土纳米颗粒界面的自旋交换和能量转移控制三重态激子

• 批准号: EP/Y015584/1
• 负责人: Akshay Rao
• 金额: $ 215.75万
• 依托单位: University of Cambridge
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2023
• 资助国家: 英国
• 起止时间: 2023 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FY015584%2F1
• 关键词: Spin; Exchange; Energy; Transfer; Hybrid

SPICE will deliver a new paradigm for the control of spin-1 triplet excitons. The starting point for SPICE is our recent discovery that in hybrid systems of organic semiconductors and lanthanide-doped inorganic nanoparticles it is possible to spin-exchange couple the molecular spin to the unpaired spins on the Ln3+ ions and to transfer energy from triplet excitons to Ln3+ and vice versa (Han et al., Nature 2020). This opens a fascinating area for exploration and discovery, as well as routes to control triplet dynamics in ways not possible via current methods.SPICE will combine steady-state and ultrafast optical spectroscopy with molecular and lanthanide nanoparticle design to explore these new phenomena and build a comprehensive mechanistic understanding of spin- exchange coupling and energy transfer at the organic-lanthanide nanoparticle interface and make proof of concept demonstrations of novel materials and device functionalities. Key aims will be:1) Building structure-function relationships to understand the mechanisms of:(a) spin-exchange mediated brightening of the normally forbidden S0-Tn transitions; (b) spin-exchange mediated enhancement of intersystem crossing (S1-T1) rates; (c) energy transfer from triplet excitons to Ln3+ and vice versa; (d) the triplet-Ln fusion process (T1+Ln-S1) to give upconverted emission and the hybrid Ln-Organic electronic states that must mediate this process.2) We will then use the insights generated to develop new materials with optimised energy transfer and emission properties.3) Finally, we will make proof of demonstrations of LEDs and optically pumped lasers with NIR emission (1300-1600nm) and NIR to blue upconversion at very low excitation powers that can trigger chemical reactions in biological environments.The success of SPICE would open new avenues to harness triplet excitons that could find transformative applications in areas ranging from photocatalysis and optoelectronics to 3D printing and optogenetics.

Spice将提供一个新的范式，以控制Spin-1三重态激子。香料的起点是我们最近发现的是，在有机半导体和泛素掺杂的无机纳米颗粒的混合系统中，可以将分子旋转到LN3+离子上的未配合的旋转以及将能量从Triplet Excitons转移到LN3+和Vice Versa（Han anda，han antaly 2020）。这为探索和发现开辟了一个迷人的领域，以及通过当前方法无法以无法进行方式控制三胞胎动态的途径。Spice将稳态和超快的光谱谱与分子和灯笼纳米粒子设计相结合，以探索这些新现象，并建立对构建型号和能量转换的全面机械的构建机械的机制，使其对有机体的互联体进行了证明，新颖的材料和设备功能。主要目的是：1）建筑结构 - 功能关系的关系，以了解以下机制：（a）自旋交换介导的正常禁止的S0-TN过渡的亮度； （b）旋转交换介导的间交叉交叉（S1-T1）速率的增强； （c）从三胞胎激子到LN3+的能量转移，反之亦然； (d) the triplet-Ln fusion process (T1+Ln-S1) to give upconverted emission and the hybrid Ln-Organic electronic states that must mediate this process.2) We will then use the insights generated to develop new materials with optimised energy transfer and emission properties.3) Finally, we will make proof of demonstrations of LEDs and optically pumped lasers with NIR emission (1300-1600nm) and NIR to blue在非常低的激发能力下，可以在生物学环境中引发化学反应的高转换。香料的成功将为线索三重态激子开放新的途径，这些途径可以在从光催化和光电分析和3D打印和光遗传学的区域中找到变革性应用。