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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.
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    Directed exciton transport highways in organic semiconductors
    ([London] : Nature Publishing Group UK, 2023) Müller, Kai; Schellhammer, Karl S.; Gräßler, Nico; Debnath, Bipasha; Liu, Fupin; Krupskaya, Yulia; Leo, Karl; Knupfer, Martin; Ortmann, Frank
    Exciton bandwidths and exciton transport are difficult to control by material design. We showcase the intriguing excitonic properties in an organic semiconductor material with specifically tailored functional groups, in which extremely broad exciton bands in the near-infrared-visible part of the electromagnetic spectrum are observed by electron energy loss spectroscopy and theoretically explained by a close contact between tightly packing molecules and by their strong interactions. This is induced by the donor–acceptor type molecular structure and its resulting crystal packing, which induces a remarkable anisotropy that should lead to a strongly directed transport of excitons. The observations and detailed understanding of the results yield blueprints for the design of molecular structures in which similar molecular features might be used to further explore the tunability of excitonic bands and pave a way for organic materials with strongly enhanced transport and built-in control of the propagation direction.