Fabrication and Characterization of Controllable Grain Boundary Arrays in Solution Processed Small Molecule Organic Semiconductor Films

TL;DR

This study demonstrates how controllable grain boundary arrays in solution-processed organic semiconductor films influence charge transport and trapping, revealing that grain boundary structure significantly impacts device mobility and trap behavior.

Contribution

It introduces a method to produce and control grain boundary arrays in organic semiconductor films, enabling systematic investigation of their effects on electronic properties.

Findings

Mobility scales with grain size, indicating grain boundaries affect charge transport.

Large-angle grain boundaries have a potential drop of over one volt.

Charge trapping is reversible and correlated with grain boundary density.

Abstract

We have produced solution-processed thin films of 6,13-bis(triisopropyl-silylethynyl) pentacene with grain sizes from a few micrometers up to millimeter scale by lateral crystallization from a rectangular stylus. Grains are oriented along the crystallization direction, and the grain size transverse to the crystallization direction depends inversely on the writing speed, hence forming a regular array of oriented grain boundaries with controllable spacing. We utilize these controllable arrays to systematically study the role of large-angle grain boundaries in carrier transport and charge trapping in thin film transistors. The effective mobility scales with the grain size, leading to an estimate of the potential drop at individual large-angle grain boundaries of more than one volt. This result indicates that the structure of grain boundaries is not molecularly abrupt, which may be a general feature of solution processed small molecule organic semiconductor thin films where relatively high energy grain boundaries are typically formed. This may be due to the crystal Transient measurements after switching from positive to negative gate bias or between large and small negative gate bias reveal reversible charge trapping with time constants on the order of 10 s, and trap densities that are correlated with grain boundary density. We suggest that charge diffusion along grain boundaries and other defects is the rate determining mechanism of the reversible trapping.