2D Molecular Crystal Bilayer p-n Junctions: A General Route toward High-Performance and Well-Balanced Ambipolar...

Ambipolar organic field-effect transistors (OFETs) are vital for the construction of high-performance all-organic digital circuits. The bilayer p-n junction structure, which is composed of separate layers of p- and n-type organic semiconductors, is considered a promising way to realize well-balanced ambipolar charge transport. However, this approach suffers from severely reduced mobility due to the rough interface between the polycrystalline thin films of p- and n-type organic semiconductors. Herein, 2D molecular crystal (2DMC) bilayer p-n junctions are proposed to construct high-performance and well-balanced ambipolar OFETs. The molecular-scale thickness of the 2DMC ensures high injection efficiency and the atomically flat surface of the 2DMC leads to high-quality p- and n-layer interfaces. Moreover, by controlling the layer numbers of the p- and n-type 2DMCs, the electron and hole mobilities are tuned and well-balanced ambipolar transport is accomplished. The hole and electron mobilities reach up to 0.87 and 0.82 cm² V^-1 s^-1 , respectively, which are the highest values among organic single-crystalline double-channel OFETs measured in ambient air. This work provides a general route to construct high-performance and well-balanced ambipolar OFETs based on available unipolar materials.