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.
Nitrogen doping is a promising method of engineering the electronic structure of a metal oxide to modify its optical and electrical properties; however, the doping effect strongly depends on the types of defects introduced. Herein, we report a comparative study of nitrogen-doping-induced defects in Cu2O. Even in the lightly doped samples, a considerable number of nitrogen interstitials (Ni) formed, accompanied by nitrogen substitutions (NO) and oxygen vacancies (VO). In the course of high-temperature annealing, these Ni atoms interacted with VO, resulting in an increase in NO and decreases in Ni and VO. The properties of the annealed sample were significantly modified as a result. Our results suggest that Ni is a significant defect type in nitrogen-doped Cu2O.
A phenomenon of wurtzite (w), zincblende (zb), and rock-salt (rs) phase separation was investigated in ZnCdO films having Cd contents in the range of 0%-60% settling a discussion on the phase stability issues in ZnCdO. First, low-Cd-content (17%) ZnCdO was realized preferentially in a w matrix determining optimal Zn-lean conditions by tuning the precursor decomposition rates during synthesis. However, more detailed analysis of x-ray diffraction and photoluminescence (PL) data revealed that the w single-phase stability range is likely to be as narrow as 0%-2% Cd, while samples containing 7%-17% of Cd exhibit a mixture of w and zb phases. Second, high-Cd-content (32%-60%) ZnCdO samples were realized, supplying more of the Cd precursor utilizing Zn-lean growth conditions, however, resulting in a mixture of w, zb, and rs phases. Characteristic PL signatures at 2.54 and 2.31 eV were attributed to zb-ZnCdO and rs-CdO, respectively, while the band gap variation in w-Zn 1−x Cd x O is given by (3.36-0.063x) as determined at 10 K. The phase separation is interpreted in terms of corresponding changes in the charge distribution and reduced stacking fault energy.
In this work we present a significant advancement in cubic silicon carbide (3C-SiC) growth in terms of crystal quality and domain size, and indicate its potential use in photovoltaics. To date, the use of 3C-SiC for photovoltaics has not been considered due to the band gap of 2.3 eV being too large for conventional solar cells. Doping of 3C-SiC with boron introduces an energy level of 0.7 eV above the valence band. Such energy level may form an intermediate band (IB) in the band gap. This IB concept has been presented in the literature to act as an energy ladder that allows absorption of sub-bandgap photons to generate extra electron-hole pairs and increase the efficiency of a solar cell. The main challenge with this concept is to find a materials system that could realize such efficient photovoltaic behavior. The 3C-SiC bandgap and boron energy level fits nicely into the concept, but has not been explored for an IB behavior.For a long time crystalline 3C-SiC has been challenging to grow due to its metastable nature. The material mainly consists of a large number of small domains if the 3C polytype is maintained. In our work a crystal growth process was realized by a new approach that is a combination of initial nucleation and step-flow growth. In the process, the domains that form initially extend laterally to make larger 3C-SiC domains, thus leading to a pronounced improvement in crystalline quality of 3C-SiC. In order to explore the feasibility of IB in 3C-SiC using boron, we have explored two routes of introducing boron impurities; ion implantation on un-doped samples and epitaxial growth on un-doped samples using pre-doped source material. The results show that 3C-SiC doped with boron is an optically active material, and thus is interesting to be further studied for IB behavior.For the ion implanted samples the crystal quality was maintained even after high implantation doses and subsequent annealing. The same was true for the samples grown with pre-doped source material, even with a high concentration of boron impurities.We present optical emission and absorption properties of as-grown and boron implanted 3C-SiC. The low-temperature photoluminescence spectra indicate the formation of optically active deep boron centers, which may be utilized for achieving an IB behavior at sufficiently high dopant concentrations. We also discuss the potential of boron doped 3C-SiC base material in a broader range of applications, such as in photovoltaics, biomarkers and hydrogen generation by splitting water.
Polymorphs are common in nature and can be stabilized by applying external pressure in materials. The pressure and strain can also be induced by the gradually accumulated radiation disorder. However, in semiconductors, the radiation disorder accumulation typically results in the amorphization instead of engaging polymorphism. By studying these phenomena in gallium oxide we found that the amorphization may be prominently suppressed by the monoclinic to orthorhombic phase transition. Utilizing this discovery, a highly oriented single-phase orthorhombic film on the top of the monoclinic gallium oxide substrate was fabricated. Exploring this system, a novel mode of the lateral polymorphic regrowth, not previously observed in solids, was detected. In combination, these data envisage a new direction of research on polymorphs in Ga 2 O 3 and, potentially, for similar polymorphic families in other materials.
Implanted atoms can affect the evolution of ion-induced defects in radiation hard materials exhibiting a high dynamic annealing and these processes are poorly understood. Here, we study the thermal evolution of structural defects in wurtzite ZnO samples implanted at room temperature with a wide range of ion species (from 11B to 209Bi) to ion doses up to 2 × 1016 cm−2. The structural disorder was characterized by a combination of Rutherford backscattering spectrometry, nuclear reaction analysis, and transmission electron microscopy, while secondary ion mass spectrometry was used to monitor the behavior of both the implanted elements and residual impurities, such as Li. The results show that the damage formation and its thermal evolution strongly depend on the ion species. In particular, for F implanted samples, a strong out-diffusion of the implanted ions results in an efficient crystal recovery already at 600 °C, while co-implantation with B (via BF2) ions suppresses both the F out-diffusion and the lattice recovery at such low temperatures. The damage produced by heavy ions (such as Cd, Au, and Bi) exhibits a two-stage annealing behavior where efficient removal of point defects and small defect clusters occurs at temperatures ∼500 °C, while the second stage is characterized by a gradual and partial annealing of extended defects. These defects can persist even after treatment at 900 °C. In contrast, the defects produced by light and medium mass ions (O, B, and Zn) exhibit a more gradual annealing with increasing temperature without distinct stages. In addition, effects of the implanted species may lead to a nontrivial defect evolution during the annealing, with N, Ag, and Er as prime examples. In general, the obtained results are interpreted in terms of formation of different dopant-defect complexes and their thermal stability.
We study structural disorder in GaN bombarded at room temperature with 1.3 keV amu−1 PFn (n = 0, 2 and 4) cluster ions. Results are compared with our previous studies of irradiation with atomic ions of different masses. An algorithm for cascade density calculations that take into account the formation of subcascades is presented. Quantitative analysis of both new and previous data shows that an increase in the cascade density above a certain critical value results in a rapid increase in the rate of planar amorphization and the rate of damage buildup in the crystal bulk. Both such rates increase with decreasing sample temperature. This threshold-like behaviour suggests an important role of nonlinear energy spikes in the formation of stable implantation disorder in GaN. We also discuss the striking difference between cascade density effects in damage buildup in different semiconductors, including GaN, ZnO and Si.
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