Breaking Fundamental Limitation of Flow-Induced Anisotropic Growth for Large-Scale and Fast Printing of Organic Single-Crystal Films.

Advanced organic electronic technologies have put forward a pressing demand for cost-effective and high-throughput fabrication of organic single-crystal films (OSCFs). However, solution-printed OSCFs are typically plagued by the existence of abundant structural defects, which pose a formidable challenge to achieving large-scale and high-performance organic electronics. Here, it is elucidated that these structural defects are mainly originated from printing flow-induced anisotropic growth, an important factor that is overlooked for too long. In light of this, a surfactant-additive printing method is proposed to effectively overcome the anisotropic growth, enabling the deposition of uniform OSCFs over the wafer scale at a high speed of 1.2 mm s-1 at room temperature. The resulting OSCF exhibits appealing performance with a high average mobility up to 10.7 cm2 V-1 s-1, which is one of the highest values for flexible organic field-effect transistor arrays. Moreover, large-scale OSCF-based flexible logic circuits, which can be bent without degradation to a radius as small as 4.0 mm and over 1000 cycles are realized. The work provides profound insights into breaking the limitation of flow-induced anisotropic growth and opens new avenues for printing large-scale organic single-crystal electronics.

Scalable Growth of Organic Single-Crystal Films via an Orientation Filter Funnel for High-Performance Transistors with Excellent Uniformity.

Organic single-crystal films (OSCFs) provide an unprecedented opportunity for the development of new-generation organic single-crystal electronics. However, crystallization of organic films is normally governed by stochastic nucleation and incoherent growth, posing a formidable challenge to grow large-sized OSCFs. Here, an "orientation filter funnel" concept is presented for the scalable growth of OSCFs with well-aligned, singly orientated crystals. By rationally designing solvent wetting/dewetting patterns on the substrate, this approach can produce seed crystals with the same crystallographic orientation and then maintain epitaxial growth of these crystals, enabling the formation of large-area OSCFs. As a result, this unique concept for crystal growth not only enhances the average mobility of organic film by 4.5-fold but also improves its uniformity of electrical properties, with a low mobility variable coefficient of 9.8%, the new lowest record among organic devices. The method offers a general and scalable route to produce OSCFs toward real-word electronic applications.