We developed a solution-processed indium oxide (In2O3) thin-film transistor (TFT) with a boron-doped peroxo-zirconium (ZrO2:B) dielectric on silicon as well as polyimide substrate at 200 °C, using water as the solvent for the In2O3 precursor. The formation of In2O3 and ZrO2:B films were intensively studied by thermogravimetric differential thermal analysis (TG-DTA), attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FT IR), high-resolution X-ray diffraction (HR-XRD), and X-ray photoelectron spectroscopy (XPS). Boron was selected as a dopant to make a denser ZrO2 film. The ZrO2:B film effectively blocked the leakage current at 200 °C with high breakdown strength. To evaluate the ZrO2:B film as a gate dielectric, we fabricated In2O3 TFTs on the ZrO2:B dielectrics with silicon substrates and annealed the resulting samples at 200 and 250 °C. The resulting mobilities were 1.25 and 39.3 cm(2)/(V s), respectively. Finally, we realized a flexible In2O3 TFT with the ZrO2:B dielectric on a polyimide substrate at 200 °C, and it successfully operated a switching device with a mobility of 4.01 cm(2)/(V s). Our results suggest that aqueous solution-processed In2O3 TFTs on ZrO2:B dielectrics could potentially be used for low-cost, low-temperature, and high-performance flexible devices.
We demonstrated solution-processed thin film transistors on a peroxo-zirconium oxide (ZrO(2)) dielectric with a maximum temperature of 350 °C. The formation of ZrO(2) films was investigated by TG-DTA, FT-IR, and XPS analyses at various temperatures. We synthesized a zirconium oxide solution by adding hydrogen peroxide (H(2)O(2)). The H(2)O(2) forms peroxo groups in the ZrO(2) film producing a dense-amorphous phase and a smooth surface film. Because of these characteristics, the ZrO(2) film successfully blocked leakage current even in annealing at 300 °C. Finally, to demonstrate that the ZrO(2) film is dielectric, we fabricated thin-film transistors (TFTs) with a solution-processed channel layer of indium zinc oxide (IZO) on ZrO(2) films at 350 °C. These TFTs had a mobility of 7.21 cm(2)/(V s), a threshold voltage (V(th)) of 3.22 V, and a V(th) shift of 1.6 V under positive gate bias stress.
Herein, we report a novel and easy strategy for fabricating solution-processed metal oxide thin-film transistors by controlling the dielectric constant of H2O through manipulation of the metal precursor solution temperature. As a result, indium zinc oxide (IZO) thin-film transistors (TFTs) fabricated from IZO solution at 4 °C can be operated after annealing at low temperatures (∼250 °C). In contrast, IZO TFTs fabricated from IZO solutions at 25 and 60 °C must be annealed at 275 and 300 °C, respectively. We also found that IZO TFTs fabricated from the IZO precursor solution at 4 °C had the highest mobility of 12.65 cm2/(V s), whereas the IZO TFTs fabricated from IZO precursor solutions at 25 and 60 °C had field-effect mobility of 5.39 and 4.51 cm2/(V s), respectively, after annealing at 350 °C. When the IZO precursor solution is at 4 °C, metal cations such as indium (In3+) and zinc ions (Zn2+) can be fully surrounded by H2O molecules, because of the higher dielectric constant of H2O at lower temperatures. These chemical complexes in the IZO precursor solution at 4 °C are advantageous for thermal hydrolysis and condensation reactions yielding a metal oxide lattice, because of their high potential energies. The IZO TFTs fabricated from the IZO precursor solution at 4 °C had the highest mobility because of the formation of many metal-oxygen-metal (M-O-M) bonds under these conditions. In these bonds, the ns-orbitals of the metal cations overlap each other and form electron conduction pathways. Thus, the formation of a high proportion of M-O-M bonds in the IZO thin films is advantageous for electron conduction, because oxide lattices allow electrons to travel easily through the IZO.
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