Revisiting the Hetero-Interface of Electrolyte/2D Materials in an Electric Double Layer Device (Small 43/2023)

Electric double layer (EDL) devices based on 2D materials have made great achievements for versatile electronic and opto-electronic applications; however, the ion dynamics and electric field distribution of the EDL at the electrolyte/2D material interface and their influence on the physical properties of 2D materials have not been clearly clarified. In this work, by using Kelvin probe force microscope and steady/transient optical techniques, the character of the EDL and its influence on the optical properties of monolayer transition metal dichalcogenides (TMDs) are probed. The potential drop, unscreened EDL potential distribution, and accumulated carriers at the electrolyte/TMD interface are revealed, which can be explained by nonlinear Thomas–Fermi theory. By monitoring the potential distribution along the channel, the evolution of the electric field-induced lateral junction in the TMD EDL transistor is accessed, giving rise to the better exploration of EDL device physics. More importantly, EDL gate-dependent carrier recombination and exciton–exciton annihilation in monolayer TMDs on lithium-ion solid state electrolyte (Li₂Al₂SiP₂TiO₁₃) are evaluated for the first time, benefiting from the understanding of the interaction between ions, carriers, and excitons. The work will deepen the understanding of the EDL for the exploitation of functional device applications.