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Item EFFECTS OF IMPURITY BAND IN HEAVILY DOPED ZnO:HCl(Elsevier, 2019) Colibaba, Gleb; Avdonin, A.; Shtepliuk, I.; Caraman, Mihail; Domagała, J.; Inculeț, IonA comparative study of properties of ZnO:HCl single crystals obtained by various methods is presented. Characterization by photoluminescence, optical and electrical measurements in the wide temperature range has allowed to analyze the energy spectra of Cl-containing stable defects in ZnO. Presence of shallow Cl donors, deeper donor complexes, incorporating several Cl atoms or stable H-Cl pairs and presence of compensating deep acceptors, attributed to VZnClO centers, are demonstrated. The presence of shallow donor impurity band, as well as strong dependence of its activation energy on the doping level is shown. The controversy of various models for estimation of this dependence is discussed. It is demonstrated, that 90% of this dependence is caused by feature of temperature dependence of Hall coefficient related to conductive impurity band, and a more correct equation for activation energy is suggested. An abnormally low efficiency of neutral impurity scattering of charge carriers and strong optical absorption in the near-IR spectral range are demonstrated and attributed to upper conductive impurity band of negatively charged donors with an extra electron.Item SINTERING HIGHLY CONDUCTIVE ZnO:HCl CERAMICS BY MEANS OF CHEMICAL VAPOR TRANSPORT REACTIONS(Elsevier, 2019) Colibaba, GlebThe features of sintering ZnO ceramics by means of chemical vapor transport (CVT) in sealed quartz chambers were investigated. CO, C, H2, HCl, HCl + H2, HCl + C, HCl + Zn and HCl + H2+ C mixtures were used as transport agents (TAs) at the 925–1070 °C temperature range. The exact thermodynamic analysis of compound CVT systems, carried out for wide temperature and loaded TA pressure ranges, was applied to establish the relation between medium composition and the characteristics of sintered materials. The advantages of some compound TAs based on HCl were shown. ZnO:HCl ceramics with a diameter of 25 mm (99 ± 1% of the initial diameter of the sintering powder), a density of 5.1 ± 0.3 g/cm3, a hardness of 2.0 ± 0.2 GPa, a resistivity of 2.4⋅10-2 Ω cm, and a controllable stoichiometric deviation, were obtained. The investigated materials have no contamination from metallic Zn, ZnCl2 or solid C. The doping efficiency of ZnO ceramics by oxides of various metals, by means of low temperature CVT reactions with ZnCl2 vapors as a TA, was calculated for oxides of all non-radioactive metals of the periodic table.Item ZnO DOPING EFFICIENCY BY MULTIVALENT METALS IN COMPLEX CVT REACTIONS(Elsevier, 2019) Colibaba, GlebThe present investigation is a theoretical study of doping efficiency of ZnO crystals grown by using compound chemical vapor transport (CVT) agents based on HCl and doped by oxides of various metals in the growth process. The thermodynamic analysis for compositions of MexOy−ZnO–ZnCl2–CO CVT systems in the closed growth chambers was carried out for oxides (MexOy) of all non-radioactive metals of the periodic table, taking into account various types of chloride species. The influence of temperature (1000–1500 K), ZnCl2 pressure (10−2−10 atm) and Zn pressure (10−5−3 atm) on the total pressure and mass transport rate of doping species (MeCln) were investigated. The possibility of increase in the doping efficiency of ZnO by MexOy + ZnCl2 + Zn CVT reactions is predicted for some multivalent metals. Some calculation results are confirmed experimentally.Item HALIDE-CARBON VAPOR TRANSPORT OF ZnO AND ITS APPLICATION PERSPECTIVES FOR DOPING WITH MULTIVALENT METALS(Elsevier, 2018) Colibaba, GlebThe growth of ZnO single crystals in closed ampoules using HCl+C mixture as a chemical vapor transport agent (TA) was studied. The influence of growth temperature, TA density, C/HCl ratio, and undercooling on the ZnO mass transport rate was investigated theoretically and experimentally. The influence of growth medium composition on the features of crystal growth, such as the minimization of growth nucleus density, the increase in the lateral growth rate of up to 1 mm per day, the suppression of the attachment effect, and stable growth of non-polar, semi-polar and polar planes of a hexagonal structure was analyzed. The structural, photoluminescent, optical and electrical properties were investigated. The doping efficiency of ZnO by oxides of metals was analyzed for various TAs and Zn pressure in the growth medium. The possibility of increase in the doping efficiency by several orders of magnitude for multivalent metals was predicted for HCl+C TA.Item HALIDE-OXIDE CARBON VAPOR TRANSPORT OF ZnO: NOVEL APPROACH FOR UNSEEDED GROWTH OF SINGLE CRYSTALS WITH CONTROLLABLE GROWTH DIRECTION(Elsevier, 2018) Colibaba, GlebThe thermodynamic analysis of using HCl + CO gas mixture as a chemical vapor transport agent (TA) for ZnO single crystal growth in closed ampoules, including 11 chemical species, is carried out for wide temperature and loaded TA pressure ranges. The advantages of HCl + CO TA for faster and more stable growth are shown theoretically in comparison with HCl, HCl + H2 and CO. The influence of the growth temperature, of the TA density, of the HCl/CO ratio, and of the undercooling on the ZnO mass transport rate was investigated theoretically and experimentally. The HCl/CO ratios favorable for the growth of m planes and (0001)Zn surface were found. It was shown that HCl + CO TA provides: (i) a rather high growth rate (up to 1.5 mm per day); (ii) a decrease of wall adhesion effect and an etch pit density down to 103 cm−2; (iii) a minimization of growth nucleus quantity down to 1; (iv) stable unseeded growth of the high crystalline quality large single crystals with a controllable preferred growth direction. The characterization by the photoluminescence spectra, the transmission spectra and the electrical properties are analyzed.