Solution coating of large-area organic semiconductor thin films with aligned single-crystalline domains

Solution coating of organic semiconductors offers great potential for achieving low-cost manufacturing of large-area and flexible electronics. However, the rapid coating speed needed for industrial-scale production poses challenges to the control of thin-film morphology. Here, we report an approach—termed fluid-enhanced crystal engineering (FLUENCE)—that allows for a high degree of morphological control of solution-printed thin films. We designed a micropillar-patterned printing blade to induce recirculation in the ink for enhancing crystal growth, and engineered the curvature of the ink meniscus to control crystal nucleation. Using FLUENCE, we demonstrate the fast coating and patterning of millimetre-wide, centimetre-long, highly aligned single-crystalline organic semiconductor thin films. In particular, we fabricated thin films of 6,13-bis(triisopropylsilylethynyl) pentacene having non-equilibrium single-crystalline domains and an unprecedented average and maximum mobilities of 8.1±1.2 cm2 V−1 s−1 and 11 cm2 V−1 s−1. FLUENCE of organic semiconductors with non-equilibrium single-crystalline domains may find use in the fabrication of high-performance, large-area printed electronics. Solution printing of organic semiconductors could in principle be scaled to industrial needs, yet attaining aligned single-crystals directly with this method has been challenging. By using a micropillar-patterned printing blade designed to enhance the control of crystal nucleation and growth, thin films of macroscopic, highly aligned single crystals of organic semiconductors can now be fabricated.