Engineering of Neutral Excitons and Exciton Complexes in Transition Metal Dichalcogenide Monolayers through External Dielectric Screening

In order to fully exploit the potential of transition metal dichalcogenide monolayers (TMD-MLs), the well-controlled creation of atomically sharp lateral heterojunctions within these materials is highly desirable. A promising approach to create such heterojunctions is the local modulation of the electronic structure of an intrinsic TMD-ML via dielectric screening induced by its surrounding materials. For the realization of this non-invasive approach, an in-depth understanding of such dielectric effects is required. We report on the modulations of excitonic transitions in TMD-MLs through the effect of dielectric environments including low-k and high-k dielectric materials. We present absolute tuning ranges as large as 37 meV for the optical band gaps of WSe2 and MoSe2 MLs and relative tuning ranges on the order of 30% for the binding energies of neutral excitons in WSe2 MLs. The findings suggest the possibility to reduce the electronic band gap of WSe2 MLs by 120 meV, paving the way towards dielectrically defined lateral heterojunctions.