Graphene-Quantum-Dots-Induced Centimeter-Sized Growth of Monolayer Organic Crystals for High-Performance Transistors

Monolayer organic crystals have attracted considerable attention due to their extraordinary optoelectronic properties. Solution self-assembly on the surface of water is an effective approach to fabricate monolayer organic crystals. However, due to the difficulties in controlling the spreading of organic solution on the water surface and the weak intermolecular interaction between the organic molecules, large-area growth of monolayer organic crystals remains a great challenge. Here, a graphene quantum dots (GQDs)-induced self-assembly method for centimeter-sized growth of monolayer organic crystals on a GQDs solution surface is reported. The spreading area of the organic solution can be readily controlled by tuning the pH value of the GQDs solution. Meanwhile, the π-π stacking interaction between the GQDs and the organic molecules can effectively reduce the nucleation energy of the organic molecules and afford a cohesive force to bond the crystals, enabling large-area growth of monolayer organic crystals. Using 2,7-didecyl benzothienobenzothiopene (C₁₀-BTBT) as an examples, centimeter-sized monolayer C₁₀-BTBT crystal with uniform molecular packing and crystal orientation is attained. Organic field-effect transistors based on the monolayer C₁₀-BTBT crystals exhibit a high mobility up to 2.6 cm² V^-1 s^-1, representing the highest mobility value for solution-assembled monolayer organic crystals. This work provides a feasible route for large-scale fabrication of monolayer organic crystals toward high-performance organic devices.