Ultrafast Carrier Dynamics in Two-Dimensional Electron Gas-like K-Doped MoS2

Abstract

Electronic interactions associated with atomic adsorbates on transition metal dichalcogenides such as MoS2 can induce massive electronic reconstruction that results in the formation of a new type of heavily doped transition metal dichalcogenide that exhibits characteristics of a two-dimensional electron gas. The impact of quantum confinement and reduced dimensionality on the carrier dynamics in such two-dimensional systems is at present not known, but is of paramount importance if they are to find application in optoelectronic devices. Here we show by a combination of angle-resolved photoemission and advanced x-ray spectroscopies that many-body interactions in reduced dimension drastically shorten carrier lifetimes to below 0.5 fs, and reveal how potassium intercalation in MoS2 forces orbital rehybridization to create a two-dimensional electron gas.