Introducing correlations into carrier transport simulations of disordered materials through seeded nucleation: impact on density of states, carrier mobility, and carrier statistics

Abstract

Disorder in organic semiconductors has made it challenging to achieve performance gains; this is a result of the many competing and often nuanced mechanisms effecting charge transport. In this article, we attempt to illuminate one of these mechanisms in the hopes of aiding experimentalists in exceeding current performance thresholds. Using a heuristic exponential function, energetic correlation has been added to the Gaussian disorder model (GDM). The new model is grounded in the concept that energetic correlations can arise in materials without strong dipoles or dopants, but may be a result of an incomplete crystal formation process. The proposed correlation has been used to explain the exponential tail states often observed in these materials; it is also better able to capture the carrier mobility field dependence, commonly known as the Poole-Frenkel dependence, when compared to the GDM. Investigation of simulated current transients shows that the exponential tail states do not necessitate Montroll and Scher fits. Montroll and Scher fits occur in the form of two distinct power law curves that share a common constant in their exponent; they are clearly observed as linear lines when the current transient is plotted using a log-log scale. Typically, these fits have been found appropriate for describing amorphous silicon and other disordered materials which display exponential tail states. Furthermore, we observe the proposed correlation function leads to domains of energetically similar sites separated by boundaries where the site energies exhibit stochastic deviation. These boundary sites are found to be the source of the extended exponential tail states, and are responsible for high charge visitation frequency, which may be associated with the molecular turnover number and ultimately the material stability.

Charge transport in the spatially correlated exponential random energy landscape: effect of the nonpositive correlation function

“…A model of the approximately exponential sDOS was suggested also by Brown and Shaheen. 47 Recently the shape of the DOS in several organic glasses serving as the popular charge transporting materials has been studied. 48 In two materials with molecules having low dipole moments ( i.e.…”

“…A model of the approximately exponential sDOS was suggested also by Brown and Shaheen. [47] Recently the shape of the DOS in several organic glasses serving as the popular charge transporting materials has been studied. [48] In two materials with molecules having low dipole moments (i.e., the very type of the materials where we can expect the dominant quadrupolar contribution to the DOS) the exponential tails of the DOS have been observed, while for materials with molecules having high dipole moments the DOS has the Gaussian shape.…”