Many-body effects beyond excitons in second-harmonic generation of monolayer MoS₂

We present a quantitative study of many-body effects including the three-particle level on second-harmonic generation in monolayer MoS _2 2 . Our approach combines many-body perturbation theory with time-dependent current-density-functional theory within an ab initio framework in the optical limit. The inclusion of two-particle excitonic effects via a dynamical long-range linear exchange-correlation kernel reproduces the qualitative features of the second-harmonic response, but differs from the experimentally reported magnitude by nearly a factor of two. By incorporating three-particle trionic correlations through a static long-range quadratic exchange-correlation kernel, we achieve significantly improved quantitative agreement with experiment for the three main bound excitonic resonances. These findings suggest that many-body interactions beyond the two-body excitonic level can play an important role in accurately describing second-order optical responses in two-dimensional semiconductors.