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    Stamping Fabrication of Flexible Planar Micro‐Supercapacitors Using Porous Graphene Inks
    (Hoboken : Wiley, 2020) Li, Fei; Qu, Jiang; Li, Yang; Wang, Jinhui; Zhu, Minshen; Liu, Lixiang; Ge, Jin; Duan, Shengkai; Li, Tianming; Bandari, Vineeth Kumar; Huang, Ming; Zhu, Feng; Schmidt, Oliver G.
    High performance, flexibility, safety, and robust integration for micro‐supercapacitors (MSCs) are of immense interest for the urgent demand for miniaturized, smart energy‐storage devices. However, repetitive photolithography processes in the fabrication of on‐chip electronic components including various photoresists, masks, and toxic etchants are often not well‐suited for industrial production. Here, a cost‐effective stamping strategy is developed for scalable and rapid preparation of graphene‐based planar MSCs. Combining stamps with desired shapes and highly conductive graphene inks, flexible MSCs with controlled structures are prepared on arbitrary substrates without any metal current collectors, additives, and polymer binders. The interdigitated MSC exhibits high areal capacitance up to 21.7 mF cm−2 at a current of 0.5 mA and a high power density of 6 mW cm−2 at an energy density of 5 µWh cm−2. Moreover, the MSCs show outstanding cycling performance and remarkable flexibility over 10 000 charge–discharge cycles and 300 bending cycles. In addition, the capacitance and output voltage of the MSCs are easily adjustable through interconnection with well‐defined arrangements. The efficient, rapid manufacturing of the graphene‐based interdigital MSCs with outstanding flexibility, shape diversity, and high areal capacitance shows great potential in wearable and portable electronics.
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    Integrated molecular diode as 10 MHz half-wave rectifier based on an organic nanostructure heterojunction
    ([London] : Nature Publishing Group UK, 2020) Li, Tianming; Bandari, Vineeth Kumar; Hantusch, Martin; Xin, Jianhui; Kuhrt, Robert; Ravishankar, Rachappa; Xu, Longqian; Zhang, Jidong; Knupfer, Martin; Zhu, Feng; Yan, Donghang; Schmidt, Oliver G.
    Considerable efforts have been made to realize nanoscale diodes based on single molecules or molecular ensembles for implementing the concept of molecular electronics. However, so far, functional molecular diodes have only been demonstrated in the very low alternating current frequency regime, which is partially due to their extremely low conductance and the poor degree of device integration. Here, we report about fully integrated rectifiers with microtubular soft-contacts, which are based on a molecularly thin organic heterojunction and are able to convert alternating current with a frequency of up to 10 MHz. The unidirectional current behavior of our devices originates mainly from the intrinsically different surfaces of the bottom planar and top microtubular Au electrodes while the excellent high frequency response benefits from the charge accumulation in the phthalocyanine molecular heterojunction, which not only improves the charge injection but also increases the carrier density.
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    On-chip integrated process-programmable sub-10 nm thick molecular devices switching between photomultiplication and memristive behaviour
    ([London] : Nature Publishing Group UK, 2022) Li, Tianming; Hantusch, Martin; Qu, Jiang; Bandari, Vineeth Kumar; Knupfer, Martin; Zhu, Feng; Schmidt, Oliver G.
    Molecular 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.