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Not All Aggregates Are Made the Same: Distinct Structures of Solution Aggregates Drastically Modulate Assembly Pathways, Morphology, and Electronic Properties of Conjugated Polymers
Advanced Materials ( IF 29.4 ) Pub Date : 2022-06-20 , DOI: 10.1002/adma.202203055
Zhuang Xu 1 , Kyung Sun Park 2 , Justin J Kwok 3 , Oliver Lin 1 , Bijal B Patel 2 , Prapti Kafle 2 , Daniel W Davies 2 , Qian Chen 1, 2, 3, 4, 5 , Ying Diao 1, 2, 3, 4, 5
Affiliation  

Tuning structures of solution-state aggregation and aggregation-mediated assembly pathways of conjugated polymers is crucial for optimizing their solid-state morphology and charge-transport property. However, it remains challenging to unravel and control the exact structures of solution aggregates, let alone to modulate assembly pathways in a controlled fashion. Herein, aggregate structures of an isoindigo–bithiophene-based polymer (PII-2T) are modulated by tuning selectivity of the solvent toward the side chain versus the backbone, which leads to three distinct assembly pathways: direct crystallization from side-chain-associated amorphous aggregates, chiral liquid crystal (LC)-mediated assembly from semicrystalline aggregates with side-chain and backbone stacking, and random agglomeration from backbone-stacked semicrystalline aggregates. Importantly, it is demonstrated that the amorphous solution aggregates, compared with semicrystalline ones, lead to significantly improved alignment and reduced paracrystalline disorder in the solid state due to direct crystallization during the meniscus-guided coating process. Alignment quantified by the dichroic ratio is enhanced by up to 14-fold, and the charge-carrier mobility increases by a maximum of 20-fold in films printed from amorphous aggregates compared to those from semicrystalline aggregates. This work shows that by tuning the precise structure of solution aggregates, the assembly pathways and the resulting thin-film morphology and device properties can be drastically tuned.

中文翻译:

并非所有的聚合体都是一样的:溶液聚合体的不同结构极大地调节了共轭聚合物的组装途径、形态和电子特性

调节共轭聚合物溶液状态聚集和聚集介导的组装途径的结构对于优化其固态形态和电荷传输性能至关重要。然而,解开和控制溶液聚集体的确切结构仍然具有挑战性,更不用说以受控方式调节组装路径了。在此,异靛蓝-联噻吩基聚合物 (PII-2T) 的聚集结构通过调节溶剂对侧链与主链的选择性来调节,这导致三种不同的组装途径:从侧链相关的无定形直接结晶聚集体,手性液晶(LC)介导的来自具有侧链和主链堆叠的半结晶聚集体的组装,以及来自主链堆叠的半结晶聚集体的随机团聚。重要的是,与半结晶的相比,无定形溶液聚集体由于弯月面引导涂层过程中的直接结晶而导致固态排列显着改善并减少了副晶无序。与半结晶聚集体相比,非晶聚集体印刷的薄膜中,由二向色比量化的排列最多可提高 14 倍,电荷载流子迁移率最多可增加 20 倍。这项工作表明,通过调整溶液聚集体的精确结构,可以大幅调整组装路径以及由此产生的薄膜形态和器件性能。由于弯月面引导的涂层过程中的直接结晶,导致显着改善的排列并减少固态的副晶紊乱。与半结晶聚集体相比,非晶聚集体印刷的薄膜中,由二向色比量化的排列最多可提高 14 倍,电荷载流子迁移率最多可增加 20 倍。这项工作表明,通过调整溶液聚集体的精确结构,可以大幅调整组装路径以及由此产生的薄膜形态和器件性能。由于弯月面引导的涂层过程中的直接结晶,导致显着改善的排列并减少固态的副晶紊乱。与半结晶聚集体相比,非晶聚集体印刷的薄膜中,由二向色比量化的排列最多可提高 14 倍,电荷载流子迁移率最多可增加 20 倍。这项工作表明,通过调整溶液聚集体的精确结构,可以大幅调整组装路径以及由此产生的薄膜形态和器件性能。与半结晶聚集体相比,非晶聚集体印刷的薄膜的电荷载流子迁移率最多增加 20 倍。这项工作表明,通过调整溶液聚集体的精确结构,可以大幅调整组装路径以及由此产生的薄膜形态和器件性能。与半结晶聚集体相比,非晶聚集体印刷的薄膜的电荷载流子迁移率最多增加 20 倍。这项工作表明,通过调整溶液聚集体的精确结构,可以大幅调整组装路径以及由此产生的薄膜形态和器件性能。
更新日期:2022-06-20
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