Long-Distance Sequential Charge Separation at Micellar Interface Mediated by Dynamic Charge Transporter: A Magnetic Field Effect Study
Long-Distance Sequential Charge Separation at Micellar Interface Mediated by Dynamic Charge Transporter: A Magnetic Field Effect Study
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DOI：
10.1021/jz502495u
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发表时间：
2015-01-15
影响因子：
5.7
通讯作者：
Ikoma, Tadaaki
中科院分区：
文献类型：
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作者：
Miura, Tomoaki;Maeda, Kiminori;Ikoma, Tadaaki
构建光生长寿命电荷分离态对于利用有机分子进行光能转换至关重要。为了实现廉价和易于制造的远距离电子转移（ET）系统，我们开发了一种利用胶束界面的超分子供体(D)发色团(C)受体(a)三元体。烷基紫素（A(2+)）吸附在Triton X-100胶束的亲水性界面上，在疏水核中携带D单元。捕获在超笼中的疏水黄素C的激发三重态会从D产生初级ET，随后从C到a（2+）产生次级ET，从而形成长寿命（bbb10 μ s）的电荷分离状态，而逃逸C的产率可以忽略不计。磁场效应分析表明，C从核心扩散到亲水性界面导致远距离ET，其电荷复合率较低，约为20%。这一动态电荷传输体的新概念对液相光子-能量转换系统的发展具有重要意义。
Construction of photogenerated long-lived charge-separated states is crucial for light-energy conversion using organic molecules. For realization of cheap and easy-to-make long-distance electron transfer (ET) systems, we have developed a supramolecular donor(D)chromophore(C)acceptor(A) triad utilizing a micellar interface. Alkyl viologen (A(2+)) is adsorbed on the hydrophilic interface of Triton X-100 micelle, which bears D units in the hydrophobic core. Excited triplet state of a hydrophobic flavin C entrapped in the supercage gives rise to primary ET from D, which is followed by the secondary ET from C to A(2+) to give the long-lived (>10 mu s) charge-separated state with negligible yield of escaped C. Analysis of magnetic field effect reveals that diffusion of C from the core to the hydrophilic interface leads to long-distance ET with a low charge recombination yield of similar to 20%. This novel concept of dynamic charge transporter has important implications for development of photon-energy conversion systems in solution phase.