A thermal atomic layer deposition (ALD) process with tetrakis(dimethylamino) titanium and H2O as reagents has been used to deposit TiO2 films on native oxide and etched InAs(100) surfaces at 200 °C. TiO2 was deposited on etched InAs(100) surface without the formation of undesirable interfacial layers. X-ray photoelectron spectroscopy (XPS) data on a series of films of increasing thickness deposited on surfaces covered with native oxide has shown that the surface arsenic oxides are removed within the first 2-3 nm of film deposition. The indium oxides, however, after an initial reduction seem to persist and increase in intensity with film thickness. For a 6.4-nm-thick TiO2 film, XPS depth profile data demonstrate an accumulation of indium oxides at the TiO2 film surface. When the topmost layer of the indium/TiO2 film is removed, then a sharp interface between the TiO2 film and the InAs substrate is detected. This observation demonstrates that the surface oxides diffuse through fairly thick TiO2 films and may subsequently be removed by reaction with the precursor and amine byproducts of the ALD reaction. These findings underscore the importance of diffusion in understanding the so-called "interface clean-up" reaction and its potential impact on the fabrication of high-quality InAs and other Group III-V-based MOS devices.