Expeditious, scalable solution growth of metal oxide films by combustion blade coating for flexible electronics

Proc Natl Acad Sci U S A. 2019 May 7;116(19):9230-9238. doi: 10.1073/pnas.1901492116. Epub 2019 Apr 19.

Abstract

Metal oxide (MO) semiconductor thin films prepared from solution typically require multiple hours of thermal annealing to achieve optimal lattice densification, efficient charge transport, and stable device operation, presenting a major barrier to roll-to-roll manufacturing. Here, we report a highly efficient, cofuel-assisted scalable combustion blade-coating (CBC) process for MO film growth, which involves introducing both a fluorinated fuel and a preannealing step to remove deleterious organic contaminants and promote complete combustion. Ultrafast reaction and metal-oxygen-metal (M-O-M) lattice condensation then occur within 10-60 s at 200-350 °C for representative MO semiconductor [indium oxide (In2O3), indium-zinc oxide (IZO), indium-gallium-zinc oxide (IGZO)] and dielectric [aluminum oxide (Al2O3)] films. Thus, wafer-scale CBC fabrication of IGZO-Al2O3 thin-film transistors (TFTs) (60-s annealing) with field-effect mobilities as high as ∼25 cm2 V-1 s-1 and negligible threshold voltage deterioration in a demanding 4,000-s bias stress test are realized. Combined with polymer dielectrics, the CBC-derived IGZO TFTs on polyimide substrates exhibit high flexibility when bent to a 3-mm radius, with performance bending stability over 1,000 cycles.

Keywords: blade coating; combustion synthesis; solution process; thin-film transistor; ultrashort annealing time.