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It has been widely recognized that surface charge in nanomaterials can significantly affect their electrical properties. In this letter, we demonstrate that polarity of surface charge on pyrene modified silicon nanowires (SiNWs) can be switched by illumination of UV light. Unlike the reported conversion method via changing the surrounding pH value, switching process reported here takes place in real-time and does not require introduction of any other chemical species. Mechanisms of the surface charge polarity switching and potential applications of such systems were discussed. [ABSTRACT FROM AUTHOR]