Raman spectroscopy and XRD methods were applied to determine the phase composition and crystal quality of copper indium sulfide (CIS) films grown by spray pyrolysis. The aim of the study was to develop a low-cost preparation technique for solar cell quality materials. The Cu/In molar ratio in spray solution (0.8-1.1) and post-deposition heat treatment conditions were taken as variables. According to XRD, KCN-etched films from Cu-rich solutions result in single phase CuInS2. The A(1) phonon modes at 290 and 300 cm(-1) Raman spectra show that CIS films deposited at 370 degrees C consisted of chalcopyrite (CH) and Cu-Au (CA) ordered phases of CuInS2. Both XRD and Raman studies showed the presence of an extra phase in as-deposited films using Cu/In=0.8-1.0, which could belong to Cu/In5S8. Thermal treatments reduced the amount of secondary phase and improved the crystallinity of the films. The heat treatment at 525 degrees C in H'S led to an increase in CH content with a decrease in the FWHM of A(1) mode. Furthermore, the rise of the quality factor (I(CH)/I(CH)+I(CA)) up to 62% was observed, indicating the forination of CuInS2 films with better crystal quality. (c) 2004 Elsevier B.V. All rights reserved.