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A low-voltage multilevel organic thin-film memory device is proposed and demonstrated for nonvolatile data storage. Charge carrier density in the storage field was tuned up to four discrete levels in pentacene organic thin-film transistor with poly(methyl methacrylate)-modified Al2O3 film as the dielectric layer through light-assisted program procedures. Charges can be stored over 1 × 104 s at room temperature. The states can be clearly distinguished after 1 × 104 write-read cycles.