Biomimetic Light-Harvesting Antenna Based on the Self-Assembly of Conjugated Polyelectrolytes Embedded within Lipid Membranes
Biomimetic Light-Harvesting Antenna Based on the Self-Assembly of Conjugated Polyelectrolytes Embedded within Lipid Membranes
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DOI：
10.1021/acsnano.6b07111
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发表时间：
2016-11-01
期刊：
影响因子：
17.1
通讯作者：
Cosa, Gonzalo
中科院分区：
文献类型：
--
作者：
Calver, Christina F.;Schanze, Kirk S.;Cosa, Gonzalo
在这里，我们报告了一种仿生捕光天线的基础上带负电荷的聚（亚苯基乙炔）共轭聚电解质组装在一个带正电荷的脂质膜支架构建的脂质1，2-二油酰基-3-三甲基铵-丙烷（DOTAP）。通过空间机制将聚合物收获的光转移到亲脂性能量受体（花青染料DiI），由于天线效应，其有效摩尔吸收增强了18倍。发现吸收放大的二碘主要是由于从聚合物的直接能量转移。聚合物之间的同质能量转移的效率，接下来探测的膜嵌入富勒烯衍生物苯基-C-61-丁酸甲酯（PCBM）作为电子受体。PCBM能够淬灭多达五种聚合物的发射，这与适量的均相转移一致。膜容纳高密度聚合物供体而不自猝灭的能力对于实现电子能量收集的成功至关重要。这项工作突出了脂质膜作为一个平台的潜力，以组织在纳米级的捕光分子实现有效的能量转移到目标发色团/陷阱。
Here we report a biomimetic light-harvesting antenna based on negatively charged poly(phenylene ethynylene) conjugated polyelectrolytes assembled within a positively charged lipid membrane scaffold constructed by the lipid 1,2-dioleoyl-3-trimethylammonium-propane (DOTAP). Light harvested by the polymers was transferred via through-space mechanisms to a lipophilic energy acceptor (the cyanine dye DiI) whose effective molar absorption was enhanced by up to 18-fold due to the antenna effect. Absorption amplification of DiI was found to be due primarily to direct energy transfer from polymers. The efficiency of homoenergy transfer among polymers was next probed by the membrane embedding fullerene derivative phenyl-C-61-butryic acid methyl ester (PCBM) acting as an electron acceptor. PCBM was able to quench the emission of up to five polymers, consistent with a modest amount of homotransfer. The ability of the membrane to accommodate a high density of polymer donors without self-quenching was crucial to the success of electronic energy harvesting achieved. This work highlights the potential of lipid membranes as a platform to organize light-harvesting molecules on the nanoscale toward achieving efficient energy transfer to a target chromophore/trap.