Strongly Electric Field Dependent Conductivity in Quantum Dot Solids

Quantum dot (QD) solids, i.e., macroscopic materials assembled from man-made nanoscopic objects, find widespread application in optoelectronic devices like light-emitting diodes and solar cells. Charge transport in these materials is typically understood as thermally activated tunneling or hopping between states that are localized on individual QDs. Here, we show that the slow relaxation that is associated with the disorder-broadened density of (localized) states leads to a strong electric field (F) dependence of the charge carrier mobility. We interpret the results in terms of an increased effective electronic temperature Teff that exceeds that of the lattice. We use a heat balance model to derive an analytical expression for Teff(F) that is similar to, and puts a physical basis under, the phenomenological expression proposed by Marianer and Shklovskii [Phys. Rev. B 46, 13100 (1992)]. We apply this model to analyze the field- and temperature-dependent conductivity in the representative model system of ZnO QDs with varying ligand length and depletion shell thickness and find (effective) localization lengths ranging from 2 to 5 nm. Both experimental and analytical results compare favorably to kinetic Monte Carlo simulations. Due to the large value of the effective localization length, the field dependence already becomes relevant at modest fields around 1–10 V/μm, that are typical for operational conditions of photovoltaic and light emitting devices based on QD solids.