We proposed a multi-scale computational framework based on a wave-packet propagation with a non-linear tight-binding Hückel model and molecular dynamics with a density functional method, and adopted the multi-scale approach to carrier transport of organic polymers showing dynamic structural fluctuations. In the tight-binding Hückel Hamiltonian, we introduced an electron–hole binding energy, the non-linear term in the present method, and investigated the influence of the electron–hole binding on the carrier mobility. We conducted wave-packet propagation for 5 ps dynamics on two kinds of polymers with 1 μm length. We found that when the electron–hole binding energy is changed from 0 to 500 meV, the carrier mobility can be changed by two orders of magnitude. We also analyzed the localization property of the wave-packet on the polymers, and found that (1) in both small and large electron–hole binding regimes, the orbital localization simply causes the decrease in carrier mobility, and (2) in an intermediate electron–hole binding regime, the orbital localization rather enhances the carrier mobility.

中文翻译：

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基于非线性紧密结合哈密顿量的π-共轭聚合物中载流子的波包多尺度模拟

我们提出了一个基于非线性紧密结合Hückel模型的波包传播和具有密度泛函方法的分子动力学的多尺度计算框架，并采用了多尺度方法来显示具有动态结构的有机聚合物载流子波动。在紧密结合的Hückel哈密顿量中，我们引入了电子-空穴结合能（本方法中的非线性项），并研究了电子-空穴结合对载流子迁移率的影响。我们对两种长度为1μm的聚合物进行了5 ps动力学的波包传播。我们发现，当电子-空穴结合能从0变为500 meV时，载流子迁移率可以改变两个数量级。我们还分析了波包在聚合物上的定位特性，