Al-doped ZnO (AZO) thin films have been prepared by mist chemical vapor deposition and magnetron sputtering. The band gap shift as a function of carrier concentration in n-type zinc oxide (ZnO) was systematically studied considering the available theoretical models. The shift in energy gap, evaluated from optical absorption spectra, did not depend on sample preparations; it was mainly related to the carrier concentrations and so intrinsic to AZO. The optical gap increased with the electron concentration approximately as ne2∕3 for ne≤4.2×1019 cm−3, which could be fully interpreted by a modified Burstein–Moss (BM) shift with the nonparabolicity of the conduction band. A sudden decrease in energy gap occurred at 5.4−8.4×1019 cm−3, consistent with the Mott criterion for a semiconductor-metal transition. Above the critical values, the band gap increased again at a different rate, which was presumably due to the competing BM band-filling and band gap renormalization effects, the former inducing a band gap widening and the latter an offsetting narrowing. The band gap narrowing (ΔEBGN) derived from the band gap renormalization effect did not show a good ne1∕3 dependence predicated by a weakly interacting electron-gas model, but it was in excellent agreement with a perturbation theory considering different many-body effects. Based on this theory a simple expression, ΔEBGN=Ane1∕3+Bne1∕4+Cne1∕2, was deduced for n-type ZnO, as well as p-type ZnO, with detailed values of A, B, and C coefficients. An empirical relation once proposed for heavily doped Si could also be used to describe well this gap narrowing in AZO.
A linear-source ultrasonic spray chemical vapor deposition method has been developed and applied to fabricate ZnMgO ternary alloy thin films on glass substrates. A water solution of zinc acetate and magnesium acetate was ultrasonically atomized to form aerosol particles of water containing the sources, and then they were supplied onto the heated substrate by a nitrogen carrier gas through a nozzle with a linear aperture to form ZnMgO films. The source concentration ratios in the water solution successfully controlled the solid composition and hence raised the band gap of ZnMgO up to 3.75 eV, keeping the optical transmission higher than 90% for the visible-light region. An UV photodetector fabricated using the ZnMgO film showed the photoresponsivity to be as high as a few A/W, suggesting that this simple and cost-effective technique is promising for fabricating ZnMgO films for various applications.
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