Theory of ultrafast exciton interaction and spectroscopy at atomically thin semiconductor monolayer/organic molecule interfaces (B12)

提出了一种在介观尺度上研究半导体/有机分子界面（TMDC：过渡金属二硫化物）光动力学的多体理论。重点研究了无机/有机杂化系统（HIOS）激子在短脉冲激发期间和之后的动力学，并描述了它们的形成、非线性相互作用和衰变作为几何、水平对准、激子-振子相互作用、无序和掺杂的函数。为此，使用HIOS- bloch方程来探索与单个组分的内部相互作用相比，电荷和激发转移的HIOS耦合相关的条件。预测的HIOS动力学用于分析时间分辨（非）线性光谱学和电子能谱。

A many body theory for the optical dynamics at TMDC-semiconductor/organic molecule interfaces (TMDC: transition metal dichalcogenide) on a mesoscopic scale is developed. The focus is on the dynamics during and after short pulse excitation of hybrid inorganic/organic system (HIOS) excitons and describes their formation, nonlinear interaction and decay as function of geometry, level alignment, exciton-vibron interaction, disorder, and doping. For this, HIOS-Bloch equations are used to explore the conditions where the HIOS coupling for charge and excitation transfer is relevant in comparison to internal interactions of the individual constituents. The predicted HIOS dynamics is used to analyze time resolved (non-)linear optical spectroscopy and in electron spectroscopy.