Selenization growth of purely single-phase, polycrystalline CuIn1-xAlxSe2 (0 <= x <= 0.26) alloy films was demonstrated using a less-hazardous metal-organic selenide, diethylselenide [(C2H5)(2)Se: DESe], by simple thermal annealing of metal precursor. Approximately 2.0 mu m thick alloy films exhibited X-ray diffraction peaks originating exclusively from the chalcopyrite structure. Transitions seen in the low temperature photoluminescence spectra were attributed to characteristic donor-acceptor pair emissions of the state-of-the-art CuIn1-xAlxSe2 photoabsorbing layers. (C) 2008 Elsevier B.V. All rights reserved.