The ultrafast dynamics of photoexcited charge carriers in condensed matter systems play an important role in optoelectronics and solar energy conversion. Yet it is challenging to understand such multidimensional dynamics at the atomic scale. Combining the real‐time time‐dependent density functional theory with fewest‐switches surface hopping scheme, we develop time‐dependent ab initio nonadiabatic molecular dynamics (NAMD) code Hefei‐NAMD to simulate the excited carrier dynamics in condensed matter systems. Using this method, we have investigated the interfacial charge transfer dynamics, the electron–hole recombination dynamics, and the excited spin‐polarized hole dynamics in different condensed matter systems. The time‐dependent dynamics of excited carriers are studied in energy, real and momentum spaces. In addition, the coupling of the excited carriers with phonons, defects and molecular adsorptions are investigated. The state‐of‐art NAMD studies provide unique insights to understand the ultrafast dynamics of the excited carriers in different condensed matter systems at the atomic scale.

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凝聚态系统中激发载流子的从头算非绝热分子动力学研究

凝聚态系统中光激发电荷载流子的超快动力学在光电和太阳能转换中起着重要作用。然而，在原子尺度上理解这样的多维动力学是具有挑战性的。结合实时时间依赖密度泛函理论和最少开关表面跳变方案，我们开发了时间依赖的从头算绝非绝热分子动力学（NAMD）代码合肥-NAMD，以模拟凝聚态系统中的激发载流子动力学。使用这种方法，我们研究了在不同凝聚态系统中的界面电荷转移动力学，电子-空穴复合动力学以及激发的自旋极化空穴动力学。在能量，实数和动量空间中研究了受激载流子随时间变化的动力学。此外，研究了激发的载流子与声子的耦合，缺陷和分子吸附。最新的NAMD研究提供了独特的见解，以了解原子尺度上不同凝聚态系统中激发载流子的超快动力学。