Making a molecular wire:: Charge and spin transport through para-phenylene oligomers

Making a molecular wire:: Charge and spin transport through para-phenylene oligomers
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DOI:
10.1021/ja0398215
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发表时间:
2004-05-05
影响因子:
15
通讯作者:
Wasielewski, MR
Wasielewski, MR
中科院分区:
化学1区
文献类型:
--
作者:
Weiss, EA;Ahrens, MJ;Wasielewski, MR

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功能分子导线是分子电子学发展的基础。通过分子的电荷传输主要通过两种机制发生,相干超交换和非相干电荷跳跃。通过超交换占主导地位的分子的电荷传输速率随距离近似呈指数下降,这排除了使用这些分子作为有效的分子导线。相比之下,电荷传输率通过分子中不相干电荷跳跃盛行应显示几乎距离无关,线状行为。我们现在能够确定每个机制如何有助于供体-桥-受体(D-B-A)系统的整体电荷传输特性,其中D =吩噻嗪(PTZ),B = p-低聚亚苯基,和A =二萘嵌苯-3,4:9,10-双(二甲酰亚胺)(PDI),通过测量系统的电荷分离状态内的两个未配对的自旋之间的相互作用,通过磁场对自由基对和三重态重组产物的产率。
Functional molecular wires are essential for the development of molecular electronics. Charge transport through molecules occurs primarily by means of two mechanisms, coherent superexchange and incoherent charge hopping. Rates of charge transport through molecules in which superexchange dominates decrease approximately exponentially with distance, which precludes using these molecules as effective molecular wires. In contrast, charge transport rates through molecules in which incoherent charge hopping prevails should display nearly distance independent, wirelike behavior. We are now able to determine how each mechanism contributes to the overall charge transport characteristics of a donor-bridge-acceptor (D-B-A) system, where D = phenothiazine (PTZ), B = p-oligophenylene, and A = perylene-3,4:9,10-bis(dicarboximide) (PDI), by measuring the interaction between two unpaired spins within the system's charge separated state via magnetic field effects on the yield of radical pair and triplet recombination product.