This paper attempts to realize unpinned high-k insulator-semiconductor interfaces on air-exposed GaAs and In0.53Ga0.47As by using the Si interface control layer (Si ICL). Al2O3 was deposited by ex situ atomic layer deposition (ALD) as the high-k insulator. By applying an optimal chemical treatment using HF acid combined with subsequent thermal cleaning below 500 degrees C in UHV, interface bonding configurations similar to those by in situ UHV process were achieved both for GaAs and InGaAs after MBE growth of the Si ICL with no trace of residual native oxide components. As compared with the MIS structures without Si ICL, insertion of Si ICL improved the electrical interface quality, a great deal both for GaAs and InGaAs, reducing frequency dispersion of capacitance, hysteresis effects and interface state density (D-it). A minimum value of D-it of 2 x 10(11) eV(-1) cm(-2) was achieved both for GaAs and InGaAs. However, the range of bias-induced surface potential excursion within the band gap was different, making formation of electron layer by surface inversion possible in InGaAs, but not possible in GaAs. The difference was explained by the disorder induced gap state (DIGS) model. (C) 2010 Elsevier B. V. All rights reserved.