Low-Temperature Synthesis of Highly Preferentially Oriented ε-Ga₂O₃ Films for Solar-Blind Detector Application

As one of the polymorphs of the gallium oxide family, ε gallium oxide (ε-Ga₂O₃) demonstrates promising potential in high-power electronic devices and solar-blind photodetection applications. However, the synthesis of pure-phase ε-Ga₂O₃ remains challenging through low-energy consumption methods, due to its metastable phase of gallium oxide. In this study, we have fabricated pure-phase and highly oriented ε-Ga₂O₃ thin films on c-plane sapphire substrates via thermal atomic layer deposition (ALD) at a low temperature of 400 °C, utilizing low-reactive trimethylgallium (TMG) as the gallium precursor and ozone (O₃) as the oxygen source. X-ray diffraction (XRD) results revealed that the in situ-grown ε-Ga₂O₃ films exhibit a preferred orientation parallel to the (002) crystallographic plane, and the pure ε phase remains stable following a post-annealing up to 800 °C, but it completely transforms into β-Ga₂O₃ once the thermal treatment temperature reaches 900 °C. Notably, post-annealing at 800 °C significantly enhanced the crystalline quality of ε-Ga₂O₃. To evaluate the optoelectronic characteristics, metal–semiconductor–metal (MSM)-structured solar-blind photodetectors were fabricated using the ε-Ga₂O₃ films. The devices have an extremely low dark current (<1 pA), a high photo-to-dark current ratio (>10⁶), a maximum responsivity (>1 A/W), and the optoelectronic properties maintained stability under varying illumination intensities. This work provides valuable insights into the low-temperature synthesis of high-quality ε-Ga₂O₃ films and the development of ε-Ga₂O₃-based solar-blind photodetectors for practical applications.