Ultrawide-bandgap semiconductors are ushering in the next generation of high-power electronics. The correct crystal orientation can make or break successful epitaxy of such semiconductors. Here, it is found that single-crystalline layers of α-(AlGa)₂O₃ alloys spanning bandgaps of 5.4 to 8.6 eV can be grown by molecular beam epitaxy. The key step is found to be the use of m-plane sapphire crystal. The phase transition of the epitaxial layers from the α- to the narrower bandgap β-phase is catalyzed by the c-plane of the crystal. Because the c-plane is orthogonal to the growth front of the m-plane surface of the crystal, the narrower bandgap pathways are eliminated, revealing a route to much wider bandgap materials with structural purity. The resulting energy bandgaps of the epitaxial layers span a broad range, heralding the successful epitaxial stabilization of the largest bandgap materials family to date.

Here, we have explored the thermal stability of α-(Al,Ga)₂O₃ grown by the molecular-beam epitaxy on m-plane sapphire under high-temperature annealing conditions for various Al compositions (i.e., 0%, 46%, and 100%). Though uncapped α-Ga₂O₃ undergoes a structural phase transition to the thermodynamically stable β-phase at high temperatures, we find that an aluminum oxide cap grown by atomic layer deposition preserves the α-phase. Unlike uncapped α-Ga₂O₃, uncapped α-(Al,Ga)₂O₃ at 46% and 100% Al content remain stable at high temperatures. We quantify the evolution of the structural properties of α-Ga₂O₃, α-(Al,Ga)₂O₃, and α-Al₂O₃ and the energy bandgap of α-Ga₂O₃ up to 900 °C. Throughout the anneals, the α-Ga₂O₃ capped with aluminum oxide retains its high crystal quality, with no substantial roughening.

AlScN is attractive as a lattice-matched epitaxial barrier layer for incorporation in GaN high electron mobility transistors due to its large dielectric constant and polarization. The transport properties of polarization-induced two-dimensional (2D) electron gas of densities of ∼2×1013/cm2 formed at the AlScN–GaN interface is studied by Hall-effect measurements down to cryogenic temperatures. The 2D electron gas densities exhibit mobilities limited to ∼300 cm2/V s down to 10 K at AlScN/GaN heterojunctions. The insertion of a ∼2 nm AlN interlayer boosts the room temperature mobility by more than five times from ∼300 cm2/V s to ∼1573 cm2/V s, and the 10 K mobility by more than 20 times to ∼6980 cm2/V s at 10 K. These measurements provide guidelines to the limits of electron conductivities of these highly polar heterostructures.

We report controlled silicon doping of Ga2O3 grown in plasma-assisted molecular beam epitaxy. Adding an endplate to the Si effusion cell enables the control of the mobile carrier density, leading to over 5-orders of magnitude change in the electrical resistivity. Room temperature mobilities >100 cm2/V s are achieved, with a peak value >125 cm2/V s at a doping density of low-1017/cm3. Temperature-dependent Hall effect measurements exhibit carrier freeze out for samples doped below the Mott criterion. A mobility of 390 cm2/V s is observed at 97 K.

The evolution of surface morphology for single-crystal bulk Al-polar aluminum nitride substrates during ex situ cleaning, in situ cleaning, and subsequent homoepitaxy is investigated. Ex situ acid treatment is found to reveal atomic steps on the bulk AlN substrates. After in situ Al-assisted cleaning at high temperatures in a high vacuum environment monitored with reflection high-energy electron diffraction, cleaner atomic step edges are observed. Subsequent growth on the cleaned bulk AlN by molecular beam epitaxy is used to develop a phase-diagram for homoepitaxy on AlN single crystals. Secondary ion mass spectrometry profiles reveal high-purity epitaxial layers with undesired chemical impurity densities of Si, O, and C to be below detection limits. The grown homoepitaxial films are observed to oxidize in the ambient environment, but repeating the ex situ acid treatment again reveals atomic steps.

We compare the effectiveness of in situ thermal cleaning with that of Al-assisted cleaning of native surface oxides of bulk AlN for homoepitaxial growth by molecular beam epitaxy. Thermal deoxidation performed at $1450\hspace{0.17em}°\mathrm{C}$ in vacuum results in voids in the AlN substrate. On the other hand, Al-assisted deoxidation at $\approx 900°\mathrm{C}$ results in high-quality AlN homoepitaxy, evidenced by clean and wide atomic terraces on the surface and no extended defects at the growth interface. This study shows that Al-assisted in situ deoxidation is effective in removing native oxides on AlN, providing a clean surface to enable homoepitaxial growth of AlN and its heterostructures; furthermore, it is more attractive over thermal deoxidation, which needs to be conducted at much higher temperatures due to the strong bonding strength of native oxides on AlN.