Effect of Positional Disorders on Charge Transport in Nanocrystal Quantum Dot Thin Films

Understanding the impact of positional and energetic disorders in nanocrystal (NC) quantum dot thin films on charge transport is crucial to determine what to prioritize in terms of the synthesis and fabrication of these materials and to accelerate their development for electronics. Here, we computationally construct realistic NC thin films with different types of disorders and apply a density functional theory (DFT)-parameterized, kinetic Monte Carlo simulation to systematically study the effects of disorders on transport. We obtain statistics on the carrier transit pathways through the NC films and carrier residence times on individual NCs. This provides insights into the distribution of transit times across the thin films and the effective mobility. We conclude that the impact of positional disorders on charge transport depends on the type of disorder and how it affects the spacing between neighboring NCs. The formation of transport paths with short inter-NC distances can enhance mobility. Meanwhile, random packing (RP) of NCs and energetic disorders due to a distribution of NC sizes decreases mobility 2- to 4-fold. Because of the large reorganization energy of small NCs, increasing the electric field has little influence on the median residence time of a charge carrier on an NC; however, an electric field straightens the transport path of the charge carrier and reduces the average number of hops a carrier makes, which can slightly enhance mobility. Deep electronic trap states are especially detrimental to carrier mobility, particularly at low fields and when the films are otherwise highly ordered.