The dynamic nature of electrostatic disorder in organic mixed ionic and electronic conductors

Abstract

Charge dynamics in disordered media is described invariably assuming that the energy landscape for hopping site energy is stationary. Within the same framework, the correlation between low electronic disorder and high charge mobility is considered extremely robust, despite the emergence of materials with mixed ionic and electronic conductivity (OMIECs) that display high mobility coexisting with large disorder. We show in this work that the disorder of OMIEC polymers is highly dynamical, i.e. the on-site energy for charge transport fluctuates with a characteristic time comparable with that of electron transport. Under these conditions, the disorder of the “frozen” system is not relevant for the charge carrier, whose dynamics are instead controlled by the underlying dynamics of the material. Deep traps exist but have a finite lifetime. The combination of classical simulations and quantum chemical calculations on the nanosecond timescale seems ideal to disclose and characterise the phenomenon.