Microscopic Modeling of Pump-Probe Spectroscopy and Population Inversion in Transition Metal Dichalcogenides

Optical properties of transition metal dichalcogenide (TMD) monolayers are dominated by excitonic effects. These are significantly altered at high carrier densities, leading to energy renormalization, absorption bleaching, and even optical gain. Such effects are experimentally accessible in ultra-fast pump-probe measurements. Herein, the semiconductor Bloch equations are combined with the generalized Wannier equation to investigate the effect that excited carriers have on the excitonic properties of TMD monolayers. In particular, the dynamics of carrier occupation, energy renormalization, and absorption bleaching as well as population inversion and optical gain are investigated.