Sulfur passivation is used to electrically and chemically passivate the silicon-germanium (SiGe) surfaces before and during the atomic layer deposition (ALD) of aluminum oxide (Al2O3). The electrical properties of the interfaces were examined by variable frequency capacitance-voltage (C-V) spectroscopy. Interface compositions were determined by angle-resolved X-ray photoelectron spectroscopy (AR-XPS). The sulfur adsorbs to a large fraction of surface sites on the SiGe(0 01) surface, protecting the surface from deleterious surface reactions during processing. Sulfur passivation (a) improved the air stability of the cleaned surfaces prior to ALD, (b) increased the stability of the surface during high-temperature deposition, and (c) increased the Al2O3 ALD nucleation density on SiGe, thereby lowering the leakage current. S passivation suppressed formation of Ge-O bonds at the interface, leaving the majority of the Al2O3-SiGe interface terminated with direct Si-O-Al bonding. Published by Elsevier B.V.