Strongly Electric Field Dependent Conductivity in Quantum Dot Solids

TL;DR

This paper demonstrates that electric fields significantly influence charge mobility in quantum dot solids by increasing the effective electronic temperature, with a developed model explaining this behavior and implications for device performance.

Contribution

It introduces a heat balance model linking electric field to effective electronic temperature, explaining field-dependent conductivity in quantum dot solids.

Findings

Charge mobility depends strongly on electric field due to increased T_eff.

The model accurately describes conductivity in ZnO QDs with different ligand and shell properties.

Field effects are relevant at modest fields typical for photovoltaic devices.

Abstract

Charge transport in QD solids 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 T_eff that exceeds that of the lattice. We use a heat balance model to derive an analytical expression for T_eff (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 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 numerical simulations by kinetic Monte Carlo. Due to the large value of the effective localization length, the field dependence already becomes relevant at modest fields around 1-10 V/micron, that are typical for operational conditions of photovoltaic and light emitting devices based on quantum dot solids.