Catalytic Metal-Accelerated Crystallization of High-Performance Solution-Processed Earth-Abundant Metal Oxide Semiconductors.

As an alternative strategy for conventional high-temperature crystallization of metal oxide (MO) channel layers, the catalytic metal-accelerated crystallization (CMAC) process using a metal seed layer is demonstrated for low-temperature crystallization of solution-processed MO semiconductors. In the CMAC process, the catalytic metal layer plays the role of seed sites for initiating and accelerating the crystallization of amorphous MO films. Generally, the solution-processed crystalline-TiO2 (c-TiO2) films required high-temperature crystallization conditions (≥500-600 °C), showing low electrical performance with a high defect density. In contrast, the suggested CMAC process could effectively lower crystallization temperature of the a-TiO2 films, enabling high-quality c-TiO2 films with well-aligned anatase grains and low-defect density. The various crystalline catalytic layers were deposited over the earth-abundant n-type amorphous titanium oxide (a-TiO2) films. Also, then, the CMAC process was performed for facile low-temperature translation of solution-processed a-TiO2 to a highly crystallized state. In particular, the Al-CMAC process using the crystalline thin-aluminum (Al) catalytic metal seed layer facilitates low-temperature (≥300 °C) crystallization of the solution-processed a-TiO2 films and the fabrication of high-performance solution-processed c-TiO2 thin-film transistors with superior field-effect mobility, good on/off switching behavior, and improved operational stability.