Effect of pressure, temperature, and particle size on cold sintered ZnO for transparent thick films on polymer substrates

The role of pressure, temperature, and particle size on cold sintering of ZnO has been investigated with a view to developing transparent thick films for device applications. Coarse ZnO (∼90–250 nm, cZnO) particles exhibited equiaxed grain growth under all conditions eventually achieving grain sizes of ∼ 0.5–1.0 µm at 300°C/375 MPa. In contrast, nano-ZnO (40–80 nm, nZnO), exhibited grain growth along the c-axis with a broader grain size distribution (0.5–4 µm) at higher temperatures and pressure (300°C/375 MPa) than cZnO. The broader grain size distribution is attributed to greater dissolution for nZnO compared with cZnO coupled with redistribution of Zn acetate/acetic acid into pores. ZnO continues to dissolve and reprecipitate within the pores throughout the densification process resulting in localized, larger grain sizes. In plane grain growth normal to the pressing direction was observed at and near the sample surface particularly in nZnO, which is attributed to constrained-sintering. Some abnormal grain growth (10–20 µm) was also sporadically observed near or at the surface of nZnO (300°C/375 MPa) due to greater rates of reprecipitation as the transient solvent volatilizes adjacent to the die wall/plunger. Tape casting was used to fabricate single and multiple layers (≈30 µm) of ZnO on Kapton® to demonstrate the potential for device fabrication. Transparency was achieved by choosing cold sintering conditions (200°C/250 MPa) for nZnO that gave ∼95% relative density while restricting a majority of grain growth to <200 nm so that internal light scattering from grain boundaries was avoided.