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Herein, bandgap tuning of monoclinic (−201)‐oriented β‐(AlxGa1−x)2O3 thin films is achieved through a β‐Ga2O3/Al2O3 heterojunction by a feasible annealing process with an O2 atmosphere. During the annealing process, Al atoms of the Al2O3 substrate outdiffuse easily into the β‐Ga2O3 thin film deposited by ozone‐assisted molecular beam epitaxy (OMBE). The Al compositions in the β‐(AlxGa1−x)2O3 samples are tuned through adjusting the annealing temperature from 800 to 1300 °C and experimentally determined from the result of X‐ray photoelectron spectroscopy (XPS) measurements combined with Vegard's law. Successive Al‐composition‐gradient β‐(AlxGa1−x)2O3 thin films with controlled bandgap are constructed. On these bases, β‐Ga2O3 thin films are deposited on β‐(AlxGa1−x)2O3 (0 ≤ x ≤ 0.65) substrates through OMBE, yielding β‐Ga2O3/β‐(AlxGa1−x)2O3 (0 ≤ x ≤ 0.65) heterojunction structures, and the band offsets of this heterojunction are determined by XPS accordingly. This methodology to achieve high‐quality β‐(AlxGa1−x)2O3 thin films with adjustable Al composition and tunable band offsets of the β‐Ga2O3/β‐(AlxGa1−x)2O3 interface will provide guidance for potential strategies to develop and fabricate β‐(AlxGa1−x)2O3‐based deep‐UV photodetectors and power devices. [ABSTRACT FROM AUTHOR]

Growth mechanism and temperature of monoclinic gallium oxide (β‐Ga2O3) films grown by ozone molecular beam epitaxy (MBE) are investigated herein. Phase‐pure (2¯01) β‐Ga2O3 films can be grown on c‐plane sapphire substrates when the growth temperature exceeds 500 °C, and the grain size increases with the increase in the growth temperature. Sixfold rotational domains are obtained based on the epitaxial relationships (Ga2O3 < 010>//Al2O3<11¯00> and Ga2O3 < 102>//Al2O3 < 112¯0>). For the film grown at 700 °C, the threefold facets are observed for the first time, which are resulted from the easy‐cleaved (100) plane and rotational domains. In addition, the cathodoluminescence spectra of the β‐Ga2O3 films show that the proportion of ultraviolet emission increases with the increase in the growth temperature, which is attributed to the modulation of defect. Finally, the growth rate can be modulated by the ratio of Ga flux and ozone pressure. A reference is provided for heteroepitaxy of β‐Ga2O3 films and better understanding of the ozone MBE growth mechanism of oxides. [ABSTRACT FROM AUTHOR]