Structural and quantum chemical analysis of exciton coupling in homo- and heteroaggregate stacks of merocyanines.
Structural and quantum chemical analysis of exciton coupling in homo- and heteroaggregate stacks of merocyanines.
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DOI：
10.1038/ncomms12949
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发表时间：
2016-09-29
影响因子：
16.6
通讯作者：
Wuerthner, Frank
中科院分区：
文献类型：
--
作者：
Bialas, David;Zitzler-Kunkel, Andre;Kirchner, Eva;Schmidt, David;Wuerthner, Frank
激子耦合是至关重要的，并决定有机染料在（光）电子和光伏器件中的功能特性。在这里，我们表明，强激子耦合并不限于情况下，平等的发色团，因为通常假设。从两个双（mercury）染料相同或不同的发色团，分别获得四重染料堆栈，在极性较低的溶剂中，导致各自的均聚物和杂聚集体的二聚。通过NMR技术分配四重染料堆叠的结构，并通过单晶X射线分析明确证实。由具有两种不同发色团的双（mercury）形成的异质聚集体堆叠与包含两种相同发色团的双（mercury）的同质聚集体相比表现出显著不同的紫外/维斯吸收带。基于Kasha激子理论的扩展的量子化学分析适当地描述了这两种类型的堆叠的吸收特性，揭示了异质聚集体内不同发色团之间的强激子耦合。 有机染料之间的激子耦合对于光电和光伏器件是重要的，并且众所周知，强耦合发生在相等的发色团之间。在这里，Würthner和其他人展示了四重染料堆，这些染料堆在异质聚集体中的不同发色团之间具有强烈的激子耦合。
Exciton coupling is of fundamental importance and determines functional properties of organic dyes in (opto-)electronic and photovoltaic devices. Here we show that strong exciton coupling is not limited to the situation of equal chromophores as often assumed. Quadruple dye stacks were obtained from two bis(merocyanine) dyes with same or different chromophores, respectively, which dimerize in less-polar solvents resulting in the respective homo- and heteroaggregates. The structures of the quadruple dye stacks were assigned by NMR techniques and unambiguously confirmed by single-crystal X-ray analysis. The heteroaggregate stack formed from the bis(merocyanine) bearing two different chromophores exhibits remarkably different ultraviolet/vis absorption bands compared with those of the homoaggregate of the bis(merocyanine) comprising two identical chromophores. Quantum chemical analysis based on an extension of Kasha's exciton theory appropriately describes the absorption properties of both types of stacks revealing strong exciton coupling also between different chromophores within the heteroaggregate. Exciton coupling between organic dyes is important for opto-electronic and photovoltaic devices and it is well-known that strong coupling occurs between equal chromophores. Here, Würthner and others show quadruple dye stacks that have strong exciton coupling between different chromophores within a heteroaggregate.
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DOI：
10.1073/pnas.0610295104
发表时间：
2007-04-24
影响因子：
11.1
作者：
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影响因子：
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作者：
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