We observed high and persistent spontaneous buildup of the surface potential (SP) upon vacuum deposition of tris(8-hydroxyquinolinato) aluminum(III) (Alq(3)) on an Au substrate under dark conditions. SP determined by the Kelvin probe method reached 28 V at a thickness of 560 nm and the surface of the Alq(3) film was positively charged. We propose a model in which preferential orientation of the dipole moments of Alq(3) molecules is the origin of this buildup of the SP. The intensity of second-harmonic generation was also dramatically increased by the deposition of Alq(3) under dark conditions, which supports the notion of a buildup of dipole layers. This giant surface potential was almost completely removed by irradiation of Alq(3) molecules with visible light, and irradiation during deposition also prevented the buildup of SP. (C) 2002 American Institute of Physics.