离域动力学Monte Carlo模拟无序材料中离域增强的电荷和激子输运
Delocalised kinetic Monte Carlo for simulating delocalisation-enhanced charge and exciton transport in disordered materials
摘要：
电荷输运在高度有序的材料（带传导）或高度无序的材料（跳跃传导）中都是很好理解的。在中度无序的材料中-包括许多有机半导体-在任何极端情况下都有效的近似值都会崩溃，因此很难准确地模拟传导。特别是，描述波函数离域需要量子处理，这在缺乏周期性的无序材料中是困难的。在这里，我们提出了第一个三维模型的部分离域电荷和激子输运材料中的中间无序制度。我们的方法是基于极化子变换的Redfield理论，但克服了几个计算的障碍，通过将量子力学技术映射到动力学蒙特卡罗。我们的理论，离域动力学蒙特卡罗（dKMC），表明在中度无序材料的基本物理传输是部分离域电子状态之间的电荷跳跃。我们的研究结果揭示了为什么标准的动力学蒙特卡罗可以大大低估迁移率，即使在无序的有机半导体，即使是一个小的离域可以大大提高迁移率，以及显示三维计算捕捉重要的离域效应忽略在低维近似。
英文摘要：
Charge transport is well understood in both highly ordered materials (band conduction) or highly disordered ones (hopping conduction). In moderately disordered materials -- including many organic semiconductors -- the approximations valid in either extreme break down, making it difficult to accurately model the conduction. In particular, describing wavefunction delocalisation requires a quantum treatment, which is difficult in disordered materials that lack periodicity. Here, we present the first three-dimensional model of partially delocalised charge and exciton transport in materials in the intermediate disorder regime. Our approach is based on polaron-transformed Redfield theory, but overcomes several computational roadblocks by mapping the quantum-mechanical techniques onto kinetic Monte Carlo. Our theory, delocalised kinetic Monte Carlo (dKMC), shows that the fundamental physics of transport in moderately disordered materials is that of charges hopping between partially delocalised electronic states. Our results reveal why standard kinetic Monte Carlo can dramatically underestimate mobilities even in disordered organic semiconductors, where even a little delocalisation can substantially enhance mobilities, as well as showing that three-dimensional calculations capture important delocalisation effects neglected in lower-dimensional approximations.
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