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For what is to our knowledge the first time, electric-field-induced optical second-harmonic generation (SHG) is studied at the Si–SiO_2 interface by the use of a metal-oxide-semiconductor (MOS) structure. The crystallographic anisotropy of this phenomenon is studied for MOS structures. Experimental results indicate that the MOS technique of dc electric-field application to the Si–SiO_2 interface can be effectively used for studying electroinduced effects on SHG.