Quantum simulations of photoexcited low-dimensional systems are pivotal for understanding how to functionalize and integrate novel two-dimensional (2D) materials in next-generation optoelectronic devices. First-principles predictions are extremely challenging due to the simultaneous interplay of light-matter, electron-electron, and electron-nuclear interactions. We here present an advanced ab initio many-body method that accounts for quantum coherence and non-Markovian effects while treating electrons and nuclei on equal footing, thereby preserving fundamental conservation laws like the total energy. The impact of this advancement is demonstrated through real-time simulations of the complex multivalley dynamics in a molybdenum disulfide (MoS2) monolayer pumped above gap. Within a single framework, we provide a parameter-free description of the coherent-to-incoherent crossover, elucidating the role of microscopic and collective excitations in the dephasing and thermalization processes.
Keywords: dynamical screening; lattice heating; non-Markovian dynamics; phonon-induced decoherence; two-dimensional systems; ultrafast carrier dynamics.