Theory and Ab Initio Computation of the Anisotropic Light Emission in Monolayer Transition Metal Dichalcogenides

Abstract: Monolayer transition metal dichalcogenides (TMDCs) are direct gap semiconductors with unique potential for ultrathin light emitters. Yet, their photoluminescence (PL) is not completely understood. We compute the radiative recombination rate in monolayer TMDCs as a function of photon emission direction and polarization, and obtain polar plots of the PL for different excitation scenarios using the ab initio Bethe-Salpeter equation. We show that excitons in a quantum superposition state of the K and K' inequivalent valleys emit light anisotropically upon recombination. Our results can explain the PL anisotropy and polarization dependence measured in recent experiments, and predict new light emission regimes. When averaged over emission angle and exciton momentum, our new treatment recovers the temperature dependent radiative lifetimes we previously derived. Our work provides a first-principles approach to study light emission in two-dimensional materials.