Machine learning accelerated nonadiabatic dynamics simulations of materials with excitonic effects

Abstract

This study presents an efficient methodology for simulating nonadiabatic dynamics of complex materials with excitonic effects by integrating machine learning (ML) models with simplified Tamm–Dancoff approximation (sTDA) calculations. By leveraging ML models, we accurately predict ground-state wavefunctions using unconverged Kohn–Sham (KS) Hamiltonians. These ML-predicted KS Hamiltonians are then employed for sTDA-based excited-state calculations (sTDA/ML). The results demonstrate that excited-state energies, time-derivative nonadiabatic couplings, and absorption spectra from sTDA/ML calculations are accurate enough compared with those from conventional density functional theory based sTDA (sTDA/DFT) calculations. Furthermore, sTDA/ML-based nonadiabatic molecular dynamics simulations on two different materials systems, namely chloro-substituted silicon quantum dot and monolayer black phosphorus, achieve more than 100 times speedup than the conventional linear response time-dependent DFT simulations. This work highlights the potential of ML-accelerated nonadiabatic dynamics simulations for studying the complicated photoinduced dynamics of large materials systems, offering significant computational savings without compromising accuracy.