Quantum simulations of photoexcited low-dimensional systemsarepivotal for understanding how to functionalize and integrate noveltwo-dimensional (2D) materials in next-generation optoelectronic devices.First-principles predictions are extremely challenging due to thesimultaneous interplay of light-matter, electron-electron,and electron-nuclear interactions. We here present an advancedab initio many-body method that accounts for quantum coherence andnon-Markovian effects while treating electrons and nuclei on equalfooting, thereby preserving fundamental conservation laws like thetotal energy. The impact of this advancement is demonstrated throughreal-time simulations of the complex multivalley dynamics in a molybdenumdisulfide (MoS2) monolayer pumped above gap. Within a singleframework, we provide a parameter-free description of the coherent-to-incoherentcrossover, elucidating the role of microscopic and collective excitationsin the dephasing and thermalization processes.
Perfetto, E., Stefanucci, G. (2023). Real-Time GW-Ehrenfest-Fan-Migdal Method for Nonequilibrium 2D Materials. NANO LETTERS, 23(15), 7029-7036 [10.1021/acs.nanolett.3c01772].
Real-Time GW-Ehrenfest-Fan-Migdal Method for Nonequilibrium 2D Materials
Enrico Perfetto
;Gianluca Stefanucci
2023-01-01
Abstract
Quantum simulations of photoexcited low-dimensional systemsarepivotal for understanding how to functionalize and integrate noveltwo-dimensional (2D) materials in next-generation optoelectronic devices.First-principles predictions are extremely challenging due to thesimultaneous interplay of light-matter, electron-electron,and electron-nuclear interactions. We here present an advancedab initio many-body method that accounts for quantum coherence andnon-Markovian effects while treating electrons and nuclei on equalfooting, thereby preserving fundamental conservation laws like thetotal energy. The impact of this advancement is demonstrated throughreal-time simulations of the complex multivalley dynamics in a molybdenumdisulfide (MoS2) monolayer pumped above gap. Within a singleframework, we provide a parameter-free description of the coherent-to-incoherentcrossover, elucidating the role of microscopic and collective excitationsin the dephasing and thermalization processes.I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.
