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Identification of complex defect has been a long-sought-after physics problem for controlling the defect population and engineering the useful properties in wide bandgap oxide semiconductors. Here we report a systematic study of (GaZn-VZn)- acceptor complex defect via zinc self-diffusion in Ga-doped ZnO isotopic heterostructures, which were conceived and prepared with delicately controlled growth conditions. The secondary ion mass spectrometry and temperature-dependent Hall-effect measurements reveal that a high density of controllable (GaZn-VZn)- is the predominant compensating defect in Ga-doped ZnO. The binding energy of this complex defect obtained from zinc self-diffusion experiments (~0.78 eV) well matches the electrical activation energy derived from the temperature-dependent electrical measurements (~0.82 eV). The compensation ratios were quantitatively calculated by energetic analysis and scattering process to further validate the compensation effect of (GaZn-VZn)- complex in Ga-doped ZnO. Meanwhile, its energy level structure was suggested based on the photoluminescence spectra, and the lifetime was achieved from the time-resolved photoluminescence measurements. The electron transitions between the (GaZn-VZn)- complex defect levels emit the light at ~650 nm with a lifetime of 10-20 nanoseconds. These findings may greatly pave the way towards novel complex defects-derived optical applications.

Oxygen vacancy (VO) is a common native point defects that plays crucial roles in determining the physical and chemical properties of metal oxides such as ZnO. However, fundamental understanding of VO is still very sparse. Specifically, whether VO is mainly responsible for the n-type conductivity in ZnO has been still unsettled in the past fifty years. Here we report on a study of oxygen self-diffusion by conceiving and growing oxygen-isotope ZnO heterostructures with delicately-controlled chemical potential and Fermi level. The diffusion process is found to be predominantly mediated by VO. We further demonstrate that, in contrast to the general belief of their neutral attribute, the oxygen vacancies in ZnO are actually +2 charged and thus responsible for the unintentional n-type conductivity as well as the non-stoichiometry of ZnO. The methodology can be extended to study oxygen-related point defects and their energetics in other technologically important oxide materials., Comment: 5 figures

N-type doping of high-resistance wide bandgap semiconductors, wurtzite high-Mg-content MgxZn1-xO for instance, has always been a fundamental application-motivated research issue. Herein, we report a solution to enhancing the conductivity of high-resistance Mg0.51Zn0.49O active components, which has been reliably achieved by fluorine doping via radio-frequency plasma assisted molecular beam epitaxial growth. Fluorine dopants were demonstrated to be effective donors in Mg0.51Zn0.49O single crystal film having a solar-blind 4.43 eV bandgap, with an average concentration of 1.0E19 F/cm3.The dramatically increased carrier concentration (2.85E17 cm-3 vs ~1014 cm-3) and decreased resistivity (129 ohm.cm vs ~10E6 ohm cm) indicate that the electrical properties of semi-insulating Mg0.51Zn0.49O film can be delicately regulated by F doping. Interestingly, two donor levels (17 meV and 74 meV) associated with F were revealed by temperature-dependent Hall measurements. A Schottky type metal-semiconductor-metal ultraviolet photodetector manifests a remarkably enhanced photocurrent, two orders of magnitude higher than that of the undoped counterpart. The responsivity is greatly enhanced from 0.34 mA/W to 52 mA/W under 10 V bias. The detectivity increases from 1.89E9 cm Hz1/2/W to 3.58eE10 cm Hz1/2/W under 10 V bias at room temperature.These results exhibit F doping serves as a promising pathway for improving the performance of high-Mg-content MgxZn1-xO-based devices., Comment: 8 pages