When voltage is applied on the metal layer of a surface plasmon resonance (SPR) sensor, electric field excitation causes charge accumulation on the metal surface. This alters not only the optical properties of the metal but also the SPR angle. In this study we investigate this effectby performing experiments using solutions of various pH values, and we obtain the relation between total surface charge and SPR angle. The curves for the various pH conditions become coincident. We compare our results to those from an earlier space charge layer (SCL) model, and suggest a modified SCL model which explains our result well. This result will be useful in applications of SPR sensors, and in studying the optical properties of thin metal layers.