Quantitative Energy Transfer in Organic Nanoparticles Based on Small-Molecule Ionic Isolation Lattices for UV Light Harvesting
Quantitative Energy Transfer in Organic Nanoparticles Based on Small-Molecule Ionic Isolation Lattices for UV Light Harvesting
复制标题
基于小分子离子隔离晶格的有机纳米颗粒的紫外光采集定量能量转移
DOI：
10.1021/acsanm.2c01899
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发表时间：
2022
影响因子：
5.9
通讯作者：
Laursen, Bo W.
中科院分区：
文献类型：
--
作者：
Chen, Junsheng;Stenspil, Stine G.;Kaziannis, Spyridon;Kacenauskaite, Laura;Lenngren, Nils;Kloz, Miroslav;Flood, Amar H.;Laursen, Bo W.
基于有机染料的荧光纳米粒子是一种很有前途的生物成像材料。最近，通过将阳离子罗丹明染料与氰星阴离子受体分级共组装，得到了具有橙色发光的超亮荧光纳米颗粒，形成了小分子离子隔离晶格(SMILES)。氰星阴离子络合物提供罗丹明染料的空间和电子隔离，禁止聚集猝灭。蓝星还构成了一个紫外线激发天线系统，以提高罗丹明微笑纳米颗粒的亮度，因为它在紫外区具有较大的摩尔吸收系数，并能有效地将能量传递给染料。为了进一步研究紫外光的捕获过程，我们比较了罗丹明微笑纳米颗粒和基于青绿发光的微笑纳米颗粒，它们在氰化星和染料分子之间的光谱重叠方面有所不同。由于光谱重叠的增加，能量转移效率从罗丹明微笑的80%增加到花菁微笑纳米粒的100%。利用飞秒暂态吸收(TA)光谱详细研究了纳米粒子的能量传递过程，得到花菁和罗丹明类纳米粒子的能量传递时间常数分别约为0.4ps和1.3ps。这一结果与光谱重叠积分有很好的相关性，并解释了能量转移和紫外光收集效率的增加。这种对超分子微笑材料中紫外光能量收集过程的洞察将有助于未来超亮功能纳米材料的设计。
Fluorescent nanoparticles based on organic dyes are promising materials for bioimaging applications. Recently, ultrabright fluorescent nanoparticles with orange emission were obtained by hierarchical coassembly of a cationic rhodamine dye with cyanostar anion-receptor to produce small-molecule ionic isolation lattices (SMILES). The cyanostar anion-complexes provides spatial and electronic isolation of the rhodamine dye prohibiting aggregation quenching. Cyanostar also constitutes a UV excitation antenna system to boost the brightness of the rhodamine SMILES nanoparticles due to a large molar absorption coefficient in the UV region and efficient energy transfer to the dye. To further study the UV light harvesting process, we compared the rhodamine SMILES nanoparticles to green emissive cyanine-based SMILES nanoparticles, different in spectral overlap between cyanostar and the dye molecules. The energy transfer efficiency is increased from 80% in rhodamine SMILES to 100% in cyanine SMILES NPs due to increased spectral overlap. The energy transfer process was studied in detail by using femtosecond (fs) transient absorption (TA) spectroscopy, yielding energy transfer time-constants of around 0.4 and 1.3 ps for the cyanine- and rhodamine-based SMILES NPs, respectively. This result correlates well with the spectral overlap integrals and accounts for increased energy transfer and UV light harvesting efficiency. This insight into the UV light energy harvesting processes in the supramolecular SMILES materials will aid future design of ultrabright functional nanomaterials.
影响因子：
16.6
作者：
Huang, Yinjuan;Xing, Jie;Zhang, Qichun
通讯作者：
Zhang, Qichun