GaAs surfaces were self-cleaned through fast pulsing of the Trimethylaluminum (TMA) precursor by reducing and restraining the regrowth of native oxides using the atomic layer deposition (ALD). The thermal conversion of As-O in to Ga-O reduction was evaluated by the X-ray photoelectron spectroscopy. Metal oxide semiconductor (MOS) capacitor was using ZrO2 as high-k gate dielectric on n-GaAs substrates, and their superior performance in electrical properties has been demonstrated. ZrO2/GaAs capacitor exhibits superior capacitance-voltage characteristics reduced leakage current due to reduced interfacial trap density. These studies have remarkable significance for the development of high-throughput innovative electronics, using ZrO2 as high-k dielectric. (C) 2013 Published by Elsevier B.V.