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.
At a glance
- Large modulation of carrier transport by grain-boundary molecular packing and microstructure in organic thin films. Nature Mater. 8, 952–958 (2009). et al.
- Contact-induced crystallinity for high-performance soluble acene-based transistors and circuits. Nature Mater. 7, 216–221 (2008). et al.
- Tuning charge transport in solution-sheared organic semiconductors using lattice strain. Nature 480, 504–508 (2011). et al.
- Controlled deposition of highly ordered soluble acene thin films: Effect of morphology and crystal orientation on transistor performance. Adv. Mater. 21, 4926–4931 (2009). et al.
- A zone-casting technique for device fabrication of field-effect transistors based on discotic hexa-peri-hexabenzoeoronene. Adv. Mater. 17, 684–689 (2005). et al.
- High-performance organic thin-film transistors through solution-sheared deposition of small-molecule organic semiconductors. Adv. Mater. 20, 2588–2594 (2008). , , , &
- Anisotropic mobility in large grain size solution processed organic semiconductor thin films. Appl. Phys. Lett. 92, 063302 (2008). , , &
- Very high mobility in solution-processed organic thin-film transistors of highly ordered 1 benzothieno 3,2-b benzothiophene derivatives. Appl. Phys. Express 2, 111501 (2009). , , , &
- Controlled solution deposition and systematic study of charge-transport anisotropy in single crystal and single-crystal textured TIPS pentacene thin films. Org. Electron. 10, 696–703 (2009). , , , &
- High-mobility field-effect transistors from large-area solution- grown aligned C60 single crystals. J. Am. Chem. Soc. 134, 2760–2765 (2012). et al.
- High-performance transistors and complementary inverters based on solution-grown aligned organic single-crystals. Adv. Mater. 24, 2588–2591 (2012). et al.
- Inkjet printing of single-crystal films. Nature 475, 364–367 (2011). et al.
- Controllable growth and field-effect property of monolayer to multilayer microstripes of an organic semiconductor. J. Am. Chem. Soc. 132, 8807–8809 (2010). et al.
- Fabrication and characterization of controllable grain boundary arrays in solution-processed small molecule organic semiconductor films. J. Appl. Phys. 111, 073716 (2012). , &
- Organic single-crystal arrays from solution-phase growth using micropattern with nucleation control region. Adv. Mater. 24, 1117–1122 (2012). et al.
- Patterning organic single-crystal transistor arrays. Nature 444, 913–917 (2006). et al.
- Selective crystallization of organic semiconductors on patterned templates of carbon nanotubes. Adv. Funct. Mater. 17, 2891–2896 (2007). et al.
- Capillary flow as the cause of ring stains from dried liquid drops. Nature 389, 827–829 (1997). et al.
- Use of necked-down areas to control nucleation site and direction of solidification of polycrystalline silicon using excimer laser crystallization. J. Appl. Phys. 88, 3349–3353 (2000). &
- 1969). in X-ray Diffraction (Addison-Wesley Series in Metallurgy and Materials, Addison-Wesley,
- Quantitative determination of organic semiconductor microstructure from the molecular to device scale. Chem. Rev. 112, 5488–5519 (2012). , , , &
- Organic single-crystal field-effect transistors. Mater. Today 10, 20–27 (March, 2007). &
- Polymorph selectivity under nanoscopic confinement. J. Am. Chem. Soc. 126, 3382–3383 (2004). , , &
- Confinement of molecular liquids: Consequences on thermodynamic, static and dynamical properties of benzene and toluene. Eur. Phys. J. E 12, 19–28 (2003). et al.
- Gel-induced selective crystallization of polymorphs. J. Am. Chem. Soc. 134, 673–684 (2012). et al.
- Thermally induced solid-state phase transition of bis(triisopropylsilylethynyl) pentacene crystals. J. Phys. Chem. B 110, 16397–16403 (2006). , &
- Thin film structure of triisopropylsilylethynyl-functionalized pentacene and tetraceno 2,3-b thiophene from grazing incidence X-ray diffraction. Adv. Mater. 23, 127–131 (2011). , &
- Supplementary Information (1,767 KB)