Computational characterization of charge transport resiliency in molecular solids
Computational characterization of charge transport resiliency in molecular solids
复制标题
分子固体中电荷传输弹性的计算表征
DOI：
10.1039/d1me00163a
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发表时间：
2022
影响因子：
3.6
通讯作者：
Ganapathysubramanian, Baskar
中科院分区：
文献类型：
--
作者：
Pokuri, Balaji Sesha;Ryno, Sean M.;Noruzi, Ramin;Risko, Chad;Ganapathysubramanian, Baskar
有机半导体已在多种应用中得到应用。影响器件性能的一个关键特性是构成这些器件中活性层的分子固体的电荷传输迁移率。人们对获取、量化和理解分子固体中电荷传输迁移率对热、机械和化学扰动的恢复能力越来越感兴趣。在这里，我们将分子模拟与图形表征相结合，以量化电荷传输的弹性。我们考虑 PTB7 系统的全原子模拟，并基于早期的图形方法来快速表征 PTB7 分子模拟的电荷迁移率。我们引入图中心性度量来根据分子固体中单体对电荷传输的重要性对单体进行排序。然后，我们系统地量化“失活”越来越多的单体对整体电荷传输迁移率的影响。这提供了分子固体对增加的结构扰动量的弹性的测量。我们发现这里考虑的 PTB7 系统中的电荷传输对于从参与电荷传输中移除的大量单体具有惊人的弹性。该方法提供了一种定量方法来推断电荷传输弹性，并可用于设计弹性分子固体。
Organic semiconductors have found utility in a diverse array of applications. A key property impacting device performance is the charge transport mobility of the molecular solids making up the active layer in these devices. There is increasing interest in accessing, quantifying, and understanding the resilience of charge transport mobility to thermal, mechanical, and chemical perturbations in molecular solids. Here, we integrate molecular simulations with graph characterization to quantify the resilience of charge transport. We consider all-atom simulations of the PTB7 system and build on earlier graph approaches to rapidly characterize the charge mobility of the PTB7 molecular simulations. We introduce graph centrality measures to rank order monomers in the molecular solid in terms of their importance to charge transport. We then systematically quantify the impact of ‘deactivating’ an increasing number of monomers on the overall charge transport mobility. This provides a measure of the resiliency of the molecular solid to increasing amounts of structural perturbations. We find that charge transport in the PTB7 system considered here is surprisingly resilient to significant amounts of monomers removed from participation in charge transport. This method provides a quantitative approach to reason about charge transport resilience and can be used to design resilient molecular solids.