Pd-Porphyrin Oligomers Sensitized for Green-to-Blue Photon Upconversion: The More the Better?
Pd-Porphyrin Oligomers Sensitized for Green-to-Blue Photon Upconversion: The More the Better?
复制标题
对绿-蓝光子上转换敏感的钯-卟啉低聚物：越多越好？
DOI：
10.1002/chem.201504498
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发表时间：
2016
期刊：
影响因子：
--
通讯作者：
Li Yi
中科院分区：
文献类型：
--
作者：
Xun Zhiqing;Zeng Yi;Chen Jinping;Yu Tianjun;Zhang Xiaohui;Yang Guoqiang;Li Yi
合成了一系列直接介观连接的钯-卟啉齐聚物(PdDTP-M、PdDTP-D和PdDTP-T)。Pd-卟啉低聚物的吸收范围和捕光能力随着Pd-卟啉单元数目的增加而拓宽和增强。以钯-卟啉齐聚物为敏化剂，9，10-二苯基菲为受体，在脱氧甲苯中构建了三重态-三重态湮没上转换(TTA-UC)体系，并在532 nm激光激发下观察到了绿光到蓝光的上转换。在激发功率密度为500 mW cm(-2)时，[PdDTP-M]/DPA、[PdDTP-D]/DPA和[PdDTP-T]/DPA体系的三重态-三重态湮没上转换量子效率分别为6.2 %、10.5 %和1.6 %。详细研究了TTA-UC系统的光物理过程。在[PdDTP-D]/DPA体系中观察到的较高的三重态-三重态湮没上转换量子效率可以通过增强PdDTP-D在532 nm处的光捕获能力得到合理的解释。在相同的实验条件下，[PdDTP-D]/DPA体系比另外两个TTA-UC体系产生更多的(3)DPA*，有利于三重态-三重态的湮灭过程。本工作为利用Pd-卟啉齐聚物作为增敏剂开发高效、广谱响应的TTA-UC体系提供了一条有用的途径。
A series of directly meso-meso-linked Pd-porphyrin oligomers (PdDTP-M, PdDTP-D, and PdDTP-T) have been prepared. The absorption region and the light-harvesting ability of the Pd-porphyrin oligomers are broadened and enhanced by increasing the number of Pd-porphyrin units. Triplet-triplet annihilation upconversion (TTA-UC) systems were constructed by utilizing the Pd-porphyrin oligomers as the sensitizer and 9,10-diphenylanthracene (DPA) as the acceptor in deaerated toluene and green-to-blue photon upconversion was observed upon excitation with a 532 nm laser. The triplet-triplet annihilation upconversion quantum efficiencies were found to be 6.2 %, 10.5 %, and 1.6 % for the [PdDTP-M]/DPA, [PdDTP-D]/DPA, and [PdDTP-T]/DPA systems, respectively, under an excitation power density of 500 mW cm(-2) . The photophysical processes of the TTA-UC systems have been investigated in detail. The higher triplet-triplet annihilation upconversion quantum efficiency observed in the [PdDTP-D]/DPA system can be rationalized by the enhanced light-harvesting ability of PdDTP-D at 532 nm. Under the same experimental conditions, the [PdDTP-D]/DPA system produces more (3) DPA* than the other two TTA-UC systems, benefiting the triplet-triplet annihilation process. This work provides a useful way to develop efficient TTA-UC systems with broad spectral response by using Pd-porphyrin oligomers as sensitizers.