Band gap energy bowing and residual strain in CuAl(S _xSe _1-x) ₂ chalcopyrite semiconductor epilayers grown by low-pressure metalorganic vapor phase epitaxy

A quadratic dependence of the band gap energy on the alloy composition x was quantified for CuAl(S _xSe _1-x) ₂ films grown by low-pressure metalorganic vapor phase epitaxy, by means of photoreflectance and photoluminescence excitation spectroscopies. The bowing parameter for the A-exciton energy was estimated to be 0.20 eV. Several high-quality films grown on GaAs(001) substrates exhibited excitonic photoluminescence peaks in the blue to ultraviolet spectral ranges. The flow rate of the Al precursor was found to affect the incorporation ratio of S/Se, indicating that the Al-S compound plays a key role in controlling x. All films grown on GaAs(001) showed c(001) orientation. Conversely, the epitaxitial orientation of the films on GaP(001) changed from a(100) to c(001) with an increase in x. The critical value of x was around 0.5. The preferred orientations were explained by the natural selection rule under which the lattice strain in the epilayer is minimized. The residual strain in the 0.5-μm-thick epilayers on GaAs(001) was nearly constant for all x, although the lattice mismatch between the epilayer and the GaAs substrate varied from 0.62% to 5.39% with an increase in x. Consequently the strain was attributed to thermal stress.