Effective lifetime of non-equilibrium carriers in semiconductors from non-adiabatic molecular dynamics simulations

The lifetime of non-equilibrium electrons and holes in semiconductors is crucial for solar cell optoelectronic applications. Non-adiabatic molecular dynamics (NAMD) simulations based on time-dependent density functional theory (TDDFT) are widely used to study excited-state carrier dynamics. However, the calculated lifetimes often different from experimental results by orders magnitude. In this work, revisiting definition considering recombination mechanisms, we report a systematic procedure calculating effective realistic semiconductor crystals that can be compared directly measurements. shows all mechanisms using reasonable densities carriers defects lifetime. When NAMD consider only Shockey-Read-Hall (SRH) defect-assisted band-to-band non-radiative while neglect radiative recombination, supercell much higher than those under illumination, ineffective thus differ experiments. Using our procedure, halide perovskite CH3NH3PbI3 agrees with It mainly determined negligible. These indicate it possible calculate accurately simulations, but values should converted comparison revised applied future simulations.