The surface chemical compositions, atomic concentration percentage and layer thickness after "high-temperature" single-step activation and "high-low temperature" two-step activation were obtained using quantitative analysis of angle-dependent X-ray photoelectron spectroscopy (XPS). It was found that compared to single-step activation, the thickness of GaAs-O interface barrier had a remarkable decrease, the degree of As-O bond became much smaller and the Ga-O bond became dominating, and at the same time the thickness of (Cs, O) layer also had a deduction while the ratio of Cs to O had no change after two-step activation. The measured spectral response curves showed that a increase of 29% of sensitivity had been obtained after two-step activation. To explore the inherent mechanisms of influences of the evolution of GaAs(Cs, O) surface layers on photoemission, surface electric barrier models based on the experimental results were built. By calculation of electron escape probability it was found that the decrease of thickness of GaAs-O interface barrier and (Cs, O) layer is the main reasons, which explained why higher sensitivity is achieved after two-step activation than single-step activation. (c) 2005 Elsevier B.V. All rights reserved.