The interference colors resulting from thin films of Al2O3 deposited by atomic layer deposition (ALD) on silicon have been rigorously analyzed using a recently developed robotic gonioreflectometer. A series of eleven increasingly thick films was deposited, up to 1613 angstrom, and their reflectance values obtained for the visible spectrum. A comparison of these values with the predictions of computer simulations employing Fresnel equations has revealed that while there was generally good agreement between predicted and measured spectra, there are some spectral regions that exhibit large deviations from predicted reflectances, typically at near-normal measurement angles and shorter wavelengths. The effect of these discrepancies on color appearance was investigated in the CIE L*a*b* color space for the daylight illuminant D65. Large iridescence is both predicted and measured for most film thicknesses. Chroma and hue differences as large as 20 CIELAB units between the predicted and the measured color centers were obtained. Simulation also predicts larger iridescence than what is actually measured. A likely cause for the observed discrepancies is that the dielectric constants of the AID films deviate from the literature values for the bulk material. (C) 2011 Elsevier B.V. All rights reserved.