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The search for panchromatic light-harvesting systems: Ternary and binary antennae based on self-organised materials
Journal of Photochemistry and Photobiology A: Chemistry ( IF 4.1 ) Pub Date : 2020-08-28 , DOI: 10.1016/j.jphotochem.2020.112872
M. Santana Vega , L. Munro , D.C.A. Gowland , J. Martinelli , K. Djanashvili , F. Cucinotta

This study presents a series of light-harvesting materials, where multiple chromophores are organised into host-guest silica-micelle structures at specific locations by means of self-assembly strategies. Binary and ternary mesoscopic antennae were realized, using organometallic complexes and organic dyes as energy transfer units and varying their content and localization to manipulate transfer rate and efficiency inside the materials. Steady-state and time-resolved UV–vis spectroscopy revealed that the three-dye systems show excitation energy cascade from intramicellar dyes to a silica-grafted acceptor, with transfer efficiencies of 20–24 % per step and overall light emission spanning the whole visible range. The two-dye system reaches analogous panchromatic response, featuring almost-white light emission and 47 % efficient transfer, by exploiting the blue-green dual emission of a metallosurfactant as energy donor inside the micellar template and the red emission of a rhodamine acceptor on the silica framework. Both systems show that control over the donor-acceptor distances can be achieved to a certain extent in complex mesoscopic materials and that a vast potential is available for transfer and colour tuning, and specific use of the materials as solid-state sensitisers.



中文翻译:

寻找全色光收集系统:基于自组织材料的三元和二元天线

这项研究提出了一系列的光收集材料,其中多个发色团通过自组装策略在特定位置被组织成客体二氧化硅胶束结构。通过使用有机金属络合物和有机染料作为能量转移单元并改变其含量和位置来控制材料内部的转移速率和效率,实现了二元和三元介观天线。稳态和时间分辨紫外可见光谱显示,这三种染料系统显示出从胶束内染料到二氧化硅接枝受体的激发能级联,每步转移效率为20%至24%,并且整个可见光范围内的总发光量范围。两色系统达到类似的全色响应,具有几乎白色的发光和47%的有效转印,通过利用金属表面活性剂的蓝绿色双重发射作为胶束模板内的能量供体,以及在二氧化硅骨架上利用若丹明受体的红色发射。两种系统均表明,在复杂的介观材料中,可以在一定程度上实现对供体-受体距离的控制,并且有巨大的潜力可用于转移和颜色调节,以及将这些材料具体用作固态敏化剂。

更新日期:2020-09-23
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