Addition of the Lewis Acid Zn(C₆F₅)₂ Enables Organic Transistors with a Maximum Hole Mobility in Excess of 20 cm² V⁻¹ s⁻¹

Abstract Incorporating the molecular organic Lewis acid tris(pentafluorophenyl)borane [B(C₆F₅)₃] into organic semiconductors has shown remarkable promise in recent years for controlling the operating characteristics and performance of various opto/electronic devices, including, light‐emitting diodes, solar cells, and organic thin‐film transistors (OTFTs). Despite the demonstrated potential, however, to date most of the work has been limited to B(C₆F₅)₃ with the latter serving as the prototypical air‐stable molecular Lewis acid system. Herein, the use of bis(pentafluorophenyl)zinc [Zn(C₆F₅)₂] is reported as an alternative Lewis acid additive in high‐hole‐mobility OTFTs based on small‐molecule:polymer blends comprising 2,7‐dioctyl[1]benzothieno [3,2‐b][1]benzothiophene and indacenodithiophene–benzothiadiazole. Systematic analysis of the materials and device characteristics supports the hypothesis that Zn(C₆F₅)₂ acts simultaneously as a p‐dopant and a microstructure modifier. It is proposed that it is the combination of these synergistic effects that leads to OTFTs with a maximum hole mobility value of 21.5 cm² V⁻¹ s⁻¹. The work not only highlights Zn(C₆F₅)₂ as a promising new additive for next‐generation optoelectronic devices, but also opens up new avenues in the search for high‐mobility organic semiconductors.