Dielectric Environment-Robust Ultrafast Charge Transfer Between Two Atomic Layers

Abstract

Understanding electron transfer across two-dimensional (2D) van der Waals (vdW) interfaces especially the effect of dielectric environment not only contributes to the rational design of high performance optoelectronic and photo/electrocatalytic devices but also unravels the nature of charge motion. Herein, we investigated the electron transfer process between two atomic thin layered materials coupled by vdW force at ultimate proximity. Despite their susceptible electronic properties, we show electron transfer at 2D vdW interface is robust and ultrafast (∼30 fs), regardless of the surrounding dielectrics and solvents. Considering the static energy landscape and dynamic nuclear rearrangements, our result suggests the electronic coupling at 2D vdW heterointerfaces is sufficiently strong such that electron transfers adiabatically in a barrierless and ultrafast manner where energetics and solvent relaxation are not that relevant. The robust ultrafast electron transfer against the variation of dielectric environment is highly encouraging for 2D optoelectronic and photo/electrocatalytic devices.