Band gap and excitonic resonance energies of high-quality bulk single crystals, polycrystalline thin films, and epitaxial layers of CuInSe2 and CuGaSe2 were determined as a function of temperature by means of photoreflectance, optical absorption (OA), and photoluminescence measurements. OA spectra were fit including excitonic absorption from low temperature up to room temperature (RT). The band gap energy of 1.032 eV and free exciton (FE) resonance energy of 1.024 eV were obtained at RT for strain-free CuInSe2 giving an exciton binding energy of 7.5 meV. The band gap energy of both CuInSe2 and CuGaSe2 was found to be essentially independent of the molar ratio of Cu to group-III atom (Cu/III) for near-stoichiometric and Cu-rich samples. The disappearance of the FE absorption in the In-rich (Cu/In<0.88) CuInSe2 thin films was explained by plasma screening of Coulomb interactions. A slight decrease in the band gap energy of the In-rich films was attributed to a degradation of film quality such as high-density defects, grains, and structural disordering. The fundamental band gap energy in strained CuInSe2 and CuGaSe2 epilayers was shown to decrease due to in-plane biaxial tensile strain.

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.

Effects of an interaction between the electronic and lattice systems on the optical spectra of a wurtzite GaN epilayer were investigated. The exponentially increasing absorption tail was well explained as an Urbach–Martienssen tail, giving the characteristic phonon energy of 30 meV. The result indicates that few longitudinal optical phonons contribute to the exciton-phonon coupling even at room temperature.

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