Structural and optical study of Zn-doped As2Se3 thin films: Evidence for photoinduced formation of ZnSe nanocrystallites

Amorphous Zn-doped As2Se3 films with a nominal zinc content x up to 10 at.% were prepared by thermal evaporation. Their structure is characterized by atomic force microscopy (AFM), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), X-ray photoemission spectroscopy (XPS), and Raman spectroscopy. The AFM data show a considerable increase of the film surface roughness for films with x > 5 at.%. A strong gradient of the Zn content decreasing into the film depth is confirmed by the EDX and XPS data. Heavily Zn-doped (above 7 at.%) As2Se3 films reveal photostructural changes in the course of the Raman measurements. New Raman features are attributed to TO and LO vibrations of ZnSe nanocrystallites formed in the film under laser illumination. Depending on the laser wavelength and power density, the ZnSe nanocrystallites can experience tensile strain in the film due to a non-thermal photoplastic effect in the As2Se3 film resulting in a partial removal of the material from the laser spot. The tensile strain value, estimated from the TO and LO phonon frequency shift, is shown to reach up to 2.9 GPa.