Understanding
the crystallization mechanism of amorphous metal-oxide
thin films remains of importance to avoid the deterioration of multifunctional
flexible electronics. We derived the crystallization mechanism of
indium-based functional amorphous oxide films by using in situ X-ray
diffraction (XRD) and transmission electron microscopy (TEM) measurements.
Crystallization begins with surface nucleation, especially at low
annealing temperatures, and proceeds simultaneous nucleation and growth
in the bulk. Three-dimensional crystal growth in the film was observed
when the crystallite size was sufficiently smaller than the film thickness.
When the growing crystallites reached the film surface, the crystallization
was dominated by two- or lower-dimensional growth. Such crystallization
can be explained within the framework of the modified Avrami theory
and can be varied for tailoring the electrical properties of the amorphous
In2O3 film. After tailoring the film crystallinity
and crystallite size, the carrier mobility was improved to >100
cm2/V·s in 30 min. Our results show that a carrier
mobility
of >90 cm2/V·s can be implemented for the In2O3 film with a crystallinity of >40% and a crystallite
size of >70 nm by an optimized annealing process. The incorporation
of Ga element into amorphous In2O3 films obviously
increases the activation energy of nucleation and migration. In contrast,
Sn dopants can promote the crystal growth. This is attributed to two
kinds of migration mechanisms during the annealing in air, one of
which is the dominant migration mechanism of oxygen interstitials
in crystallized indium–tin oxide (ITO) films and the other
dominated by oxygen vacancies in In2O3 and IGO
films. Combining the modified Avrami theory with TEM observations,
we predicted the structural evolution kinetics for indium-based amorphous
oxide films and gained new insights for understanding the temporal
structure–functionality relationship during crystallization.