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Donor-Acceptor-Collector Ternary Crystalline Films for Efficient Solid-State Photon Upconversion
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2018-06-25 , DOI: 10.1021/jacs.8b04542
Taku Ogawa 1 , Masanori Hosoyamada 1 , Brett Yurash 2 , Thuc-Quyen Nguyen 2 , Nobuhiro Yanai 1, 3 , Nobuo Kimizuka 1
Affiliation  

It is pivotal to achieve efficient triplet-triplet annihilation based photon upconversion (TTA-UC) in the solid-state for enhancing potentials of renewable energy production devices. However, the UC efficiency of solid materials is largely limited by low fluorescence quantum yields that originate from the aggregation of TTA-UC chromophores and also by severe back energy transfer from the acceptor singlet state to the singlet state of the triplet donor in the condensed state. In this work, to overcome these issues, we introduce a highly fluorescent singlet energy collector as the third component of donor-doped acceptor crystalline films, in which dual energy migration, i.e., triplet energy migration for TTA-UC and succeeding singlet energy migration for transferring energy to a collector, takes place. To demonstrate this scheme, a highly fluorescent singlet energy collector was added as the third component of donor-doped acceptor crystalline films. An anthracene-based acceptor containing alkyl chains and a carboxylic moiety is mixed with the triplet donor Pt(II) octaethylporphyrin (PtOEP) and the energy collector 2,5,8,11-tetra- tert-butylperylene (TTBP) in solution, and simple spin-coating of the mixed solution gives acceptor films of nanofibrous crystals homogeneously doped with PtOEP and TTBP. Interestingly, delocalized singlet excitons in acceptor crystals are found to diffuse effectively over the distance of ∼37 nm. Thanks to this high diffusivity, only 0.5 mol % of doped TTBP can harvest most of the singlet excitons, which successfully doubles the solid-state fluorescent quantum yield of acceptor/TTBP blend films to 76%. Furthermore, since the donor PtOEP and the collector TTBP are separately isolated in the nanofibrous acceptor crystals, the singlet back energy transfer from the collector to the donor is effectively avoided. Such efficient singlet energy collection and inhibited back energy transfer processes result in a large increase of UC efficiency up to 9.0%, offering rational design principles toward ultimately efficient solid-state upconverters.

中文翻译:

用于高效固态光子上转换的供体-受体-收集器三元晶体薄膜

在固态中实现基于三重态-三重态湮灭的高效光子上转换(TTA-UC)对于增强可再生能源生产设备的潜力至关重要。然而,固体材料的 UC 效率在很大程度上受到源自 TTA-UC 发色团聚集的低荧光量子产率以及从受体单线态到凝聚态三线态供体单线态的严重反向能量转移的限制. 在这项工作中,为了克服这些问题,我们引入了一种高荧光单线态能量收集器作为供体掺杂受体晶体薄膜的第三组分,其中双能量迁移,即 TTA-UC 的三线态能量迁移和后续的单线态能量迁移将能量转移到收集器,发生。为了演示这个方案,添加了高荧光单线态能量收集器作为供体掺杂受体晶体薄膜的第三组分。含有烷基链和羧基部分的蒽基受体与三线态供体 Pt(II) 八乙基卟啉 (PtOEP) 和能量收集器 2,5,8,11-四叔丁基苝 (TTBP) 在溶液中混合,和混合溶液的简单旋涂得到均匀掺杂有 PtOEP 和 TTBP 的纳米纤维晶体的受体膜。有趣的是,发现受主晶体中的离域单线态激子在~37 nm 的距离内有效扩散。由于这种高扩散率,只有 0.5 mol% 的掺杂 TTBP 可以收集大部分单线态激子,这成功地将受体/TTBP 混合薄膜的固态荧光量子产率翻了一番,达到 76%。此外,由于供体PtOEP和集电极TTBP在纳米纤维受体晶体中分别隔离,有效避免了从集电极到供体的单线态背能量转移。这种高效的单线态能量收集和抑制反向能量转移过程导致 UC 效率大幅提高高达 9.0%,为最终高效的固态上变频器提供了合理的设计原则。
更新日期:2018-06-25
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