Intermediate polaronic charge transport in organic crystals from a many-body first-principles approach
Intermediate polaronic charge transport in organic crystals from a many-body first-principles approach
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DOI：
10.1038/s41524-022-00742-6
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发表时间：
2022-04-11
影响因子：
9.7
通讯作者：
Bernardi, Marco
中科院分区：
文献类型：
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作者：
Chang, Benjamin K.;Zhou, Jin-Jian;Bernardi, Marco
有机分子晶体中的电荷输运通常分为两种限制性机制：以弱电子-声子（e-ph）相互作用为特征的能带输运和由强e-ph相互作用形成的局域极化子引起的电荷跳跃。然而，在这两种极限情况之间，存在一种不太好理解的中间状态，其中存在极化子，但不通过跳跃进行传输。在这里，我们展示了一个多体第一性原理的方法，可以准确地预测在这个中间政权的载流子迁移率，并阐明其微观起源。我们的方法结合了有限温度累积量方法来描述强e-ph相互作用与绿色久保运输计算。我们将此无参数框架应用于萘晶体，在100和300 K之间的实验范围内展示了1.5-2倍的电子迁移率预测。我们的分析揭示了形成一个广泛的极化子卫星峰的电子光谱函数和失败的玻尔兹曼方程在中间制度。
Charge transport in organic molecular crystals (OMCs) is conventionally categorized into two limiting regimes - band transport, characterized by weak electron-phonon (e-ph) interactions, and charge hopping due to localized polarons formed by strong e-ph interactions. However, between these two limiting cases there is a less well understood intermediate regime where polarons are present but transport does not occur via hopping. Here we show a many-body first-principles approach that can accurately predict the carrier mobility in this intermediate regime and shed light on its microscopic origin. Our approach combines a finite-temperature cumulant method to describe strong e-ph interactions with Green-Kubo transport calculations. We apply this parameter-free framework to naphthalene crystal, demonstrating electron mobility predictions within a factor of 1.5-2 of experiment between 100 and 300 K. Our analysis reveals the formation of a broad polaron satellite peak in the electron spectral function and the failure of the Boltzmann equation in the intermediate regime.