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高效电子隧穿控制导电聚合物-绝缘体混合物中的输运。

Efficient Electronic Tunneling Governs Transport in Conducting Polymer-Insulator Blends.

作者信息

Keene Scott T, Michaels Wesley, Melianas Armantas, Quill Tyler J, Fuller Elliot J, Giovannitti Alexander, McCulloch Iain, Talin A Alec, Tassone Christopher J, Qin Jian, Troisi Alessandro, Salleo Alberto

机构信息

Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States.

Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States.

出版信息

J Am Chem Soc. 2022 Jun 15;144(23):10368-10376. doi: 10.1021/jacs.2c02139. Epub 2022 Jun 6.

DOI:10.1021/jacs.2c02139
PMID:35658455
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9204759/
Abstract

Electronic transport models for conducting polymers (CPs) and blends focus on the arrangement of conjugated chains, while the contributions of the nominally insulating components to transport are largely ignored. In this work, an archetypal CP blend is used to demonstrate that the chemical structure of the non-conductive component has a substantial effect on charge carrier mobility. Upon diluting a CP with excess insulator, blends with as high as 97.4 wt % insulator can display carrier mobilities comparable to some pure CPs such as polyaniline and low regioregularity P3HT. In this work, we develop a single, multiscale transport model based on the microstructure of the CP blends, which describes the transport properties for all dilutions tested. The results show that the high carrier mobility of primarily insulator blends results from the inclusion of aromatic rings, which facilitate long-range tunneling (up to 3 nm) between isolated CP chains. This tunneling mechanism calls into question the current paradigm used to design CPs, where the solubilizing or ionically conducting component is considered electronically inert. Indeed, optimizing the participation of the nominally insulating component in electronic transport may lead to enhanced electronic mobility and overall better performance in CPs.

摘要

导电聚合物(CPs)及其共混物的电子传输模型主要关注共轭链的排列,而名义上绝缘的组分对传输的贡献在很大程度上被忽略。在这项工作中,我们使用一种典型的CP共混物来证明非导电组分的化学结构对电荷载流子迁移率有重大影响。在用过量绝缘体稀释CP时,绝缘体含量高达97.4 wt%的共混物的载流子迁移率可与某些纯CP(如聚苯胺和低区域规整度的P3HT)相媲美。在这项工作中,我们基于CP共混物的微观结构开发了一个单一的多尺度传输模型,该模型描述了所有测试稀释度下的传输特性。结果表明,主要由绝缘体组成的共混物具有高载流子迁移率是由于其中包含芳香环,这有利于孤立CP链之间的长程隧穿(长达3 nm)。这种隧穿机制对当前用于设计CPs的范式提出了质疑,在该范式中,增溶或离子导电组分被认为是电子惰性的。事实上,优化名义上绝缘的组分在电子传输中的参与度可能会提高CPs的电子迁移率并总体上带来更好的性能。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1394/9204759/4364d7a9a299/ja2c02139_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1394/9204759/592754a52ee5/ja2c02139_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1394/9204759/1fd733ed9b35/ja2c02139_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1394/9204759/b71b87bfc28e/ja2c02139_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1394/9204759/9a38bc7839e7/ja2c02139_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1394/9204759/4364d7a9a299/ja2c02139_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1394/9204759/592754a52ee5/ja2c02139_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1394/9204759/1fd733ed9b35/ja2c02139_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1394/9204759/b71b87bfc28e/ja2c02139_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1394/9204759/9a38bc7839e7/ja2c02139_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1394/9204759/4364d7a9a299/ja2c02139_0006.jpg

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