Topology-Mediated Enhanced Polaron Coherence in Covalent Organic Frameworks,The Journal of Physical Chemistry Letters

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Topology-Mediated Enhanced Polaron Coherence in Covalent Organic Frameworks
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2021-09-23 , DOI: 10.1021/acs.jpclett.1c02454
Raja Ghosh ₁ , Francesco Paesani ₁

Affiliation

We employ the Holstein model for polarons to investigate the relationship among defects, topology, Coulomb trapping, and polaron delocalization in covalent organic frameworks (COFs). We find that intrasheet topological connectivity and π-column density can override disorder-induced deep traps and significantly enhance polaron migration by several orders of magnitude in good agreement with recent experimental observations. The combination of percolation networks and micropores makes trigonal COFs ideally suited for charge transport followed by kagome/tetragonal and hexagonal structures. By comparing the polaron spectral signatures and coherence numbers of large three-dimensional frameworks having a maximum of 180 coupled chromophores, we show that controlling nanoscale defects and the location of the counteranion is critical for the design of new COF-based materials yielding higher mobilities. Our analysis establishes design strategies for enhanced conductivity in COFs that can be readily generalized to other classes of conductive materials such as metal–organic frameworks and perovskites.

中文翻译：

共价有机框架中拓扑介导的增强极化子相干性

我们采用极化子的荷斯坦模型来研究共价有机框架 (COF) 中缺陷、拓扑、库仑俘获和极化子离域之间的关系。我们发现片内拓扑连接和 π 柱密度可以克服无序引起的深陷阱，并显着增强极化子迁移几个数量级，与最近的实验观察结果非常一致。渗流网络和微孔的结合使三角形 COF 非常适合电荷传输，然后是 Kagome/四方和六方结构。通过比较具有最多 180 个耦合发色团的大型三维框架的极化子光谱特征和相干数，我们表明，控制纳米级缺陷和反阴离子的位置对于设计新的基于 COF 的材料产生更高的迁移率至关重要。我们的分析建立了增强 COF 导电性的设计策略，可以很容易地推广到其他类别的导电材料，如金属有机骨架和钙钛矿。

更新日期：2021-10-07

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