The
emergent ferroelectric property of κ-Ga2O3 is expected to deliver advanced functional memory and ultralow-loss
transistors, while the commonly observed rotational domains in κ-Ga2O3 make the origin of ferroelectricity mysterious.
In this work, the single-domain heteroepitaxy of orthorhombic κ-Ga2O3 epilayers on sapphire has been demonstrated
by the halide vapor-phase epitaxy (HVPE) technique. The optimal temperature
of 550 °C is energetically favorable for the stabilization of
κ-Ga2O3 on sapphire without impurity phases,
and the growth dynamics is dominated by the surface-reaction-limited
mechanism. The evolution of microstructures and optical characteristics
indicate that the κ–β phase transition
occurs at an elevated temperature of over 575 °C together with
a remarkable reduction of growth rate. With proper phase engineering,
the single-domain κ-Ga2O3 epilayers have been ultimately achieved, exhibiting multisteps resembling
a terrace morphology, a relatively low screw dislocation density of
5.2 × 107 cm–2, and reduced band
tail subgap states. The single-domain structure of orthorhombic κ-Ga2O3 was identified by the XRD ϕ-scans and
transmission electron microscopic analysis. The realization of single-domain
epitaxy allows one to uncover the driving force for the intriguing
ferroelectric behavior of κ-Ga2O3 and
to design power devices with improved performance.