Growth of single crystal, oriented SnO2 nanocolumn arrays by aerosol chemical vapour deposition

A single-step, template-free aerosol chemical vapor deposition (ACVD) method is demonstrated to grow well-aligned SnO2 nanocolumn arrays. The ACVD system parameters, which control thin film morphologies, were systematically explored to gain a qualitative understanding of nanocolumn growth mechanisms. Key growth variables include feed rates, substrate temperature, and deposition time. System dynamics relating synthesis variables to aerosol characteristics and processes (collision and sintering) are elucidated. By adjusting system parameters, control of the aspect ratio, height, and crystal structure of columns is demonstrated. A self-catalyzed (SnO2 particles) vapor-solid (VS) growth mechanism, whereby a vapor-particle deposition regime results in the formation of nanocrystals that act as nucleation sites for the preferential formation and growth of nanocolumns, is proposed and supported. Density functional theory (DFT) calculations indicate that the preferential orientation of thin films is a function of the system redox conditions, further supporting the proposed VS growth mechanism. When taken together, these results provide quantitative insight into the growth mechanism(s) of SnO2 nanocolumn thin films via ACVD, which is critical for engineering these, and other, nanostructured films for direct incorporation into functional devices.