CC BY 4.0 UnportedLi, TianmingHantusch, MartinQu, JiangBandari, Vineeth KumarKnupfer, MartinZhu, FengSchmidt, Oliver G.2022-07-132022-07-132022https://oa.tib.eu/renate/handle/123456789/9724https://doi.org/10.34657/8762Molecular devices constructed by sub-10 nm thick molecular layers are promising candidates for a new generation of integratable nanoelectronic applications. Here, we report integrated molecular devices based on ultrathin copper phthalocyanine/fullerene hybrid layers with microtubular soft-contacts, which exhibit process-programmable functionality switching between photomultiplication and memristive behaviour. The local electric field at the interface between the polymer bottom electrode and the enclosed molecular channels modulates the ionic-electronic charge interaction and hence determines the transition of the device function. When ions are not driven into the molecular channels at a low interface electric field, photogenerated holes are trapped as electronic space charges, resulting in photomultiplication with a high external quantum efficiency. Once mobile ions are polarized and accumulated as ionic space charges in the molecular channels at a high interface electric field, the molecular devices show ferroelectric-like memristive switching with remarkable resistive ON/OFF and rectification ratios.enghttps://creativecommons.org/licenses/by/4.0/500Self-assembledMonolayersNarrow-bandNanocomposite hotodetectorPolymer PhotodetectorsJunctionsGainInterfaceSmechanismDynamicsFutureArticle