论文标题
由分子内三重式三个歼灭驱动的无扩散光子上转换
Diffusion-free photon upconversion driven by intramolecular triplet-triplet annihilation in engineered conjugated chromophores
论文作者
论文摘要
基于敏化三重式三个歼灭（STTA-UC）的光子上转换是一种自旋机制，用于恢复共轭系统中暗三重状态的能量。在此过程中，通过属于不同扩散分子的两个低能三联体的碰撞和融合，产生了高能荧光单元。它在低激发强度和非固定光下的溶液中出色的产量突出了STTA-UC在太阳能技术方面的突破的巨大潜力。但是，其扩散限制的双分子性质限制了其在固态中的效率。为了克服这个问题，我们设计了一个能够同时托管多个三胞胎的分子系统，从而实现了无扩散的分子内TTA。我们通过定制的光致发光光谱实验获得了分子内三重融合的第一个直接演示，从而为实现新的单分子UpConventer家族开辟了道路，通过访问天然三重态能量储量，具有巨大的太阳能和闪电技术潜力。
The photon upconversion based on sensitized triplet-triplet annihilation (sTTA-UC) is a spin-flip mechanism exploited to recover the energy of dark triplet states in conjugated systems. In this process a high-energy fluorescent singlet is created through the collision and fusion of two low-energy triplets belonging to different diffusing molecules. Its excellent yield in solution under low excitation intensity and non-coherent light highlighted the huge potential of sTTA-UC to provide a breakthrough in solar technologies. However, its diffusion-limited bi-molecular nature limits its efficiency in the solid state. To overcome this issue, we designed a molecular systems able to host simultaneously more than one triplet, thus enabling a diffusion-free intramolecular TTA. We obtain the first direct demonstration of intramolecular triplet fusion by tailored photoluminescence spectroscopy experiments, thus opening the way to realize a new family of single molecule upconverters with huge potential in solar and lightening technologies by accessing the natural triplets energy reservoir.
