Processing-dependent thermal stability of a prototypical amorphous metal oxide

Abstract

Amorphous metal oxides (AMOs) are important candidate materials for fabricating next-generation thin-film transistors. While much attention has been directed toward the synthesis and electrical properties of AMOs, less is known about growth conditions that allow AMOs to retain their desirable amorphous state when subjected to high operating temperatures. Using in situ x-ray scattering and level-set simulations, we explore the time evolution of the crystallization process for a set of amorphous $\mathrm{I}{\mathrm{n}}_{2}{\mathrm{O}}_{3}$ thin films synthesized by pulsed-laser deposition at deposition temperatures (${T}_{d}$) of \ensuremath{-}50, \ensuremath{-}25, and 0 \ifmmode^\circ\else\textdegree\fi{}C. The films were annealed isothermally and the degree of crystallinity was determined by a quantitative analysis of the time-evolved x-ray scattering patterns. As expected, for films grown at the same ${T}_{d}$, an increase in the annealing temperature ${T}_{A}$ led to a shorter delay prior to the onset of crystallization, and a faster crystallization rate. Moreover, when lowering the deposition temperature by 25 \ifmmode^\circ\else\textdegree\fi{}C, a 40 \ifmmode^\circ\else\textdegree\fi{}C increase in annealing temperature is needed to achieve the same time interval for the crystals to grow from 10 to 90% volume fraction of the sample. Films grown at ${T}_{d}=0{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$ exhibited strong cubic texture after crystallization. A level-set method was employed to quantitatively model the texture that develops in the microstructures and to determine key parameters, such as the interface growth velocity, the nucleation density, and the activation energy. The differences observed in the crystallization processes are attributed to the changes in the atomic structure of the oxide and possible nanocrystalline inclusions that formed during the deposition of the amorphous phase.