文献类型：期刊文献

英文题名：Dodecaborane-Based Dopants Designed to Shield Anion Electrostatics Lead to Increased Carrier Mobility in a Doped Conjugated Polymer

作者：Aubry, Taylor J.[1];Axtell, Jonathan C.[1];Basile, Victoria M.[1];Winchell, K. J.[1];Lindemuth, Jeffrey R.[2];Porter, Tyler M.[3];Liu, Ji-Yuan[1,4,5];Alexandrova, Anastassia N.[1,6];Kubiak, Clifford P.[3];Tolbert, Sarah H.[1,6,7];Spokoyny, Alexander M.[1,6];Schwartz, Benjamin J.[1,6]

机构：[1]Univ Calif Los Angeles, Dept Chem & Biochem, Los Angeles, CA 90095 USA;[2]Lake Shore Cryotron, Westerville, OH 43082 USA;[3]Univ Calif San Diego, Dept Chem & Biochem, La Jolla, CA 92093 USA;[4]East China Univ Sci & Technol, Key Lab Adv Mat, Ctr Computat Chem, Shanghai 200237, Peoples R China;[5]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[6]Univ Calif Los Angeles, Calif NanoSyst Inst, Los Angeles, CA 90095 USA;[7]Univ Calif Los Angeles, Dept Mat Sci & Engn, Los Angeles, CA 90095 USA

年份：2019

卷号：31

期号：11

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20190506437694);WOS:【SCI-EXPANDED(收录号:WOS:000461575300007)】；

基金：This work was supported by the National Science Foundation under awards CHE-1608957 and CBET-1510353. The authors thank Alex I. Wixtrom and Miles Savage for assistance with synthesis of DDB-F72. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. J.-Y.L. thanks the CSC Fellowship. A.N.A. thanks the NSF CAREER Award CHE-1351968. TD-DFT calculations were performed using Extreme Science and Engineering Discovery Environment's (XSEDE) computing resources. A.M.S. thanks 3M Non-tenured Faculty Award, Alfred P. Sloan Foundation (Fellowship in Chemistry), and Research Corporation for Science Advancement (Cottrell Scholar).

语种：英文

外文关键词：Coulomb screening; dodecaboranes; molecular dopants; mobility; semiconducting polymers

摘要：One of the most effective ways to tune the electronic properties of conjugated polymers is to dope them with small-molecule oxidizing agents, creating holes on the polymer and molecular anions. Undesirably, strong electrostatic attraction from the anions of most dopants localizes the holes created on the polymer, reducing their mobility. Here, a new strategy utilizing a substituted boron cluster as a molecular dopant for conjugated polymers is employed. By designing the cluster to have a high redox potential and steric protection of the core-localized electron density, highly delocalized polarons with mobilities equivalent to films doped with no anions present are obtained. AC Hall effect measurements show that P3HT films doped with these boron clusters have conductivities and polaron mobilities roughly an order of magnitude higher than films doped with F-4 TCNQ, even though the boron-cluster-doped films have poor crystallinity. Moreover, the number of free carriers approximately matches the number of boron clusters, yielding a doping efficiency of approximate to 100%. These results suggest that shielding the polaron from the anion is a critically important aspect for producing high carrier mobility, and that the high polymer crystallinity required with dopants such as F-4 TCNQ is primarily to keep the counterions far from the polymer backbone.