Cyanide treatment, which includes the immersion of Si in KCN solutions followed by a rinse, effectively passivates interface states at Si/SiO 2 interfaces by the reaction of CN - ions with interface states to form Si-CN bonds. X-ray photoelectron spectroscopy (XPS) measurements show that the concentration of the CN species in the surface region after the cyanide treatment is ~0.25 at.%. Take-off angle-dependent measurements of the XPS spectra indicate that the concentration of the CN species increases with the depth from the Si/SiO 2 interface at least up to ~2 nm when ultrathin SiO 2 layers are formed at 450 o C after the cyanide treatment. When the cyanide treatment is applied to metal-oxide-semiconductor (MOS) solar cells with <ITO/SiO 2 /n-Si> structure, the photovoltage greatly increases, leading to a high conversion efficiency of 16.2% in spite of the simple cell structure with no pn-junction. Si-CN bonds are not ruptured by air mass 1.5 100 mWcm - 2 irradiation for 1000 h, and consequently the solar cells show no degradation. Neither are Si-CN bonds broken by heat treatment at 800 o C performed after the cyanide treatment. The thermal and irradiation stability of the cyanide treatment is attributable to strong Si-CN bonds, whose bond energy is calculated to be 1 eV higher than that of the Si-H bond energy using a density functional method.