CuIn1-xAlxSe2 thin films are investigated for their application as the absorber layer material for high efficiency solar cells. Single-phase CuIn1-xAlxSe2 films were deposited by four source elemental evaporation with a composition range of 0less than or equal toxless than or equal to0.6. All these films demonstrate a normalized subband gap transmission >85% with 2 mum film thickness. Band gaps obtained from spectroscopic ellipsometry show an increase with the Al content in the CuIn1-xAlxSe2 film with a bowing parameter of 0.62. The structural properties investigated using x-ray diffraction measurements show a decrease in lattice spacing as the Al content increases. Devices with efficiencies greater than 10% are fabricated on CuIn1-xAlxSe2 material over a wide range of Al composition. The best device demonstrated 11% efficiency, and the open circuit voltage increases to 0.73 V. (C) 2002 American Institute of Physics.