Optical absorption spectra of CuInSe2 single crystals were measured for the samples with −0.150≤x≤0.053, where x represents a degree of nonstoichiometry in the formula Cu1−xIn1+xSe2. The Urbach’s tail was observed for all samples between 90 K and room temperature. The Urbach’s energy, which represents an arbitrary intensity of exciton–phonon interaction, was almost constant for the Cu-rich samples (x<0), while it increased with increasing In composition for the In-rich ones (x≳0). Such an increase of the Urbach’s energy was explained to be due to enhanced electronic distortion caused by the compositional deviation from stoichiometry in terms of simultaneous influence of electron–phonon interaction and structural disorder.

Thin polycrystalline films of Cu(In,Ga)Se2 alloy with the single-phase chalcopyrite structure were successfully grown by the chemical spray pyrolysis (CSP) method on a glass substrate at 360 and 400°C. Alloy composition in the film was well controlled by that in the spray solution. The films were characterized by X-ray diffraction, optical absorption, Raman spectroscopy, van der Pauw measurement and scanning electron microscopy. It was found that lattice constants, the optical band-gap energy and the A 1 mode phonon frequency changed continuously with the alloy composition x. A grain size of about 1 µm was obtained for Cu-rich films.

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