论文标题
乙烯:间隔者混合物显示出放热的单线裂变可连贯进行,而吸热裂变则不连贯
Acene:spacer blends show exothermic singlet fission to proceed coherently, while endothermic fission proceeds incoherently
论文作者
论文摘要
在有机材料中,单线激子裂解成三重态具有巨大的技术希望,但是由于缺乏对其复杂的辐射物质的了解,这种现象的合理应用受到阻碍。在这里,我们使用四烯和五苯薄膜中的间隔分子对空缺的受控引入作为调谐参数,以补充实验可观察到的可观察到的可观察到的可观察原理。时间分辨的光谱测量与显微镜建模相结合,使我们能够证明不同的情况,这是由于不同的单曲线到三曲线的能量比对而产生的。对于放热裂变,为五苯烯发现,光激发单线和三重态对之间的相干混合是通过振动共振来促进的,振动共振驱动裂变过程,对空位浓度的敏感性很小。对于四烯等吸热材料,这种振动共振的不可能使裂变完全不连贯。该过程显示出随空位浓度而放慢速度的过程。
The fission of singlet excitons into triplet pairs in organic materials holds great technological promise, but the rational application of this phenomenon is hampered by a lack of understanding of its complex photophysics. Here, we use the controlled introduction of vacancies by means of spacer molecules in tetracene and pentacene thin films as a tuning parameter complementing experimental observables to identify the operating principles of different singlet fission pathways. Time-resolved spectroscopic measurements in combination with microscopic modelling enables us to demonstrate distinct scenarios, resulting from different singlet-to-triplet energy alignments. For exothermic fission, as found for pentacene, coherent mixing between the photoexcited singlet and triplet pair states is promoted by vibronic resonances, which drives the fission process with little sensitivity to the vacancy concentration. For endothermic materials, such as tetracene, the impossibility of such vibronic resonances renders fission fully incoherent; a process that is shown to slow down with vacancy concentration.