AI 中文总结
研究电荷传输从原子结构预测的难题，提出无参数框架从第一性原理计算传输，通过非微扰格林 - 库博动力学揭示传输机制，推翻DNTT微观机制，给出二维传输图及设计原则，突出菲族的前景。
AI 中文摘要
电荷传输对有机晶体管和光伏器件至关重要，但从原子结构预测它仍具挑战。电子 - 声子相互作用频率、强度和空间范围各异，共同产生非微扰载流子动力学。现有方法通过假设机制或简化耦合来处理，我们引入无参数框架，从第一性原理电子 - 声子哈密顿量计算传输，用全声子谱在数百分子域中传播载流子，让传输机制和瓶颈从非微扰格林 - 库博动力学中出现。在五个代表性晶体中，该框架捕捉到了测量的迁移率、温度指数和光导率指纹。结果推翻了DNTT的主流微观机制，揭示其瞬态定位源于声子的相关在位无序而非独立跳跃波动。所得二维传输图提供了设计原则，并突出了以高迁移率并五苯为例的菲族这一未充分探索的有前景方向。
英文摘要
Charge transport governs organic transistors and photovoltaics, yet predicting it from atomic structure remains challenging. Electron--phonon interactions span disparate frequencies, strengths and spatial ranges, and collectively generate nonperturbative carrier dynamics. Existing methods regain tractability only by assuming a mechanism or reducing electron--phonon coupling to a few modes. We introduce a parameter-free framework that instead computes transport from ab initio electron--phonon Hamiltonians, propagating carriers across hundreds-of-molecule domains with the full phonon spectrum and letting transport regimes and bottlenecks emerge from nonperturbative Green--Kubo dynamics. Across five representative crystals, it captures measured mobilities, temperature exponents, and optical-conductivity fingerprints. Our results overturn the prevailing microscopic mechanism for DNTT, tracing its transient localization to correlated on-site disorder from acoustic phonons rather than independent hopping fluctuations. The resulting two-axis transport map provides design principles and highlights the underexplored phenacene family, exemplified by the high-mobility picene, as a promising direction.
