Efforts
to design and realize exotic metastable phases
with advanced
characteristics have been ongoing. However, the challenge lies in
identifying their atomic structures and synthetic routes, as most
explorations of metastability have relied on intuitions and trial-and-error
approaches. Here, we present a computational workflow based on density
functional theory (DFT) to rationalize the design of metastable materials.
We demonstrate that plasma-enhanced atomic layer deposition (PEALD)
is a profitable method for synthesizing target material. By screening
the various hypothetical crystal structures of IZO compounds, we have
identified the c-axis aligned hexagonal (CAH) In2Zn4O7 as a promising candidate due to its metastability
and superior electrical properties compared to a binary metal oxide
system. Remarkably, this metastable phase can be synthesized at a
significant temperature of 200 °C, compared to the typical crystallization
temperature of the IZO system. This low-temperature crystallization
is attributed to the distinctive features of PEALD, including tunable
atomic order, precise composition control, and adjustable plasma source.
By implementing CAH-IZO in thin-film transistor (TFT) applications,
we observed desirable characteristics, such as a μFE of 43.4
cm2/V s, despite the low indium (In) content. We believe
that this combined approach of PEALD and computational processing
can expedite the realization of novel metastable materials, with the
potential to expand their applications beyond traditionally explored
materials.