Publications by authors named "Karl Leo"

The global rise in electronic waste is alarming, driven by the persistent use of glass, epoxy, and plastic substrates owing to their cost, stability, flexibility, and transparency. This underscores the need for biodegradable alternatives with similar properties. This study shows that leaf-derived lignocellulose scaffolds can stabilize bio-sourced, solution-processed polymers by acting as natural sequestering media.

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Typically, organic solar cells (OSCs) and photodetectors (OPDs) comprise an electron donating and accepting material to facilitate efficient charge carrier generation. This approach has proven successful in achieving high-performance devices but has several drawbacks for upscaling and stability. This study presents a fully vacuum-deposited single-component OPD, employing the neat oligothiophene derivative DCV2-5T in the photoactive layer.

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Organic electrochemical transistors (OECTs) underpin a range of emerging technologies, from bioelectronics to neuromorphic computing, owing to their unique coupling of electronic and ionic charge carriers. In this context, various OECT systems exhibit significant hysteresis in their transfer curve, which is frequently leveraged to achieve non-volatility. Meanwhile, a general understanding of its physical origin is missing.

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Intermolecular charge-transfer (CT) states are extended excitons with a charge separation on the nanometer scale. Through absorption and emission processes, they couple to the ground state. This property is employed both in light-emitting and light-absorbing devices.

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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.

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Organic semiconductors have opened up many new electronic applications, enabled by properties like flexibility, low-cost manufacturing, and biocompatibility, as well as improved ecological sustainability due to low energy use during manufacturing. Most current devices are made of highly disordered thin-films, leading to poor transport properties and, ultimately, reduced device performance as well. Here, we discuss techniques to prepare highly ordered thin-films of organic semiconductors to realize fast and highly efficient devices as well as novel device types.

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The relaxation of the above-gap ("hot") carriers in lead halide perovskites (LHPs) is important for applications in photovoltaics and offers insights into carrier-carrier and carrier-phonon interactions. However, the role of quantum confinement in the hot carrier dynamics of nanosystems is still disputed. Here, we devise a single approach, ultrafast pump-push-probe spectroscopy, to study carrier cooling in six different size-controlled LHP nanomaterials.

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We demonstrate the key role of charge-transfer complexes in surface doping as a successful methodology for improving channel field-effect mobility and reducing the threshold voltage in organic field-effect transistors (OFETs), as well as raising the film conductivity. Demonstrated here for 2,7-dioctyl[1]benzothieno[3,2-][1]benzothiophene (C-BTBT) doped with 2,2'-(perfluoronaphthalene-2,6-diylidene)dimalononitrile (FTCNNQ), channel doping by sequential deposition is consistently rationalized by the development of a cocrystalline structure that forms and evolves from the surface of the organic semiconductor film without trading the thin-film structure integrity. This scenario brings higher benefits for the device operation than doping by codeposition, where a decrease in the field-effect mobility of the device, even for a dopant content of only 1 mol %, makes codeposition less suitable.

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Wavelength-discriminating systems typically consist of heavy benchtop-based instruments, comprising diffractive optics, moving parts, and adjacent detectors. For simple wavelength measurements, such as lab-on-chip light source calibration or laser wavelength tracking, which do not require polychromatic analysis and cannot handle bulky spectroscopy instruments, lightweight, easy-to-process, and flexible single-pixel devices are attracting increasing attention. Here, a device is proposed for monotonously transforming wavelength information into the time domain with room-temperature phosphorescence at the heart of its functionality, which demonstrates a resolution down to 1 nm and below.

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Despite their increasing usefulness in a wide variety of applications, organic electrochemical transistors still lack a comprehensive and unifying physical framework able to describe the current-voltage characteristics and the polymer/electrolyte interactions simultaneously. Building upon thermodynamic axioms, we present a quantitative analysis of the operation of organic electrochemical transistors. We reveal that the entropy of mixing is the main driving force behind the redox mechanism that rules the transfer properties of such devices in electrolytic environments.

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A comprehensive study of the optical properties of CsPbBr perovskite multiple quantum wells (MQW) with organic barrier layers is presented. Quantum confinement is observed by a blue-shift in absorption and emission spectra with decreasing well width and agrees well with simulations of the confinement energies. A large increase of emission intensity with thinner layers is observed, with a photoluminescence quantum yield up to 32 times higher than that of bulk layers.

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Devices made using thin-film semiconductors have attracted much interest recently owing to new application possibilities. Among materials systems suitable for thin-film electronics, organic semiconductors are of particular interest; their low cost, biocompatible carbon-based materials and deposition by simple techniques such as evaporation or printing enable organic semiconductor devices to be used for ubiquitous electronics, such as those used on or in the human body or on clothing and packages. The potential of organic electronics can be leveraged only if the performance of organic transistors is improved markedly.

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We investigate the charge and thermoelectric transport in modulation-doped large-area rubrene thin-film crystals with different crystal phases. We show that modulation doping allows achieving superior doping efficiencies even for high doping densities, when conventional bulk doping runs into the reserve regime. Modulation-doped orthorhombic rubrene achieves much improved thermoelectric power factors, exceeding 20 μW m K at 80°C.

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Highly responsive organic photodetectors allow a plethora of applications in fields like imaging, health, security monitoring, etc. Photomultiplication-type organic photodetectors (PM-OPDs) are a desirable option due to their internal amplification mechanism. However, for such devices, significant gain and low dark currents are often mutually excluded since large operation voltages often induce high shot noise.

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Efficient external radiation is essential for solar cells to achieve high power conversion efficiency (PCE). The classical limit of 1/2 (, refractive index) for electroluminescence quantum efficiency (ELQE) has recently been approached by perovskite solar cells (PSCs). Photon recycling (PR) and light scattering can provide an opportunity to surpass this limit.

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Omnipresent quality monitoring in food products, blood-oxygen measurement in lightweight conformal wrist bands, or data-driven automated industrial production: Innovation in many fields is being empowered by sensor technology. Specifically, organic photodetectors (OPDs) promise great advances due to their beneficial properties and low-cost production. Recent research has led to rapid improvement in all performance parameters of OPDs, which are now on-par or better than their inorganic counterparts, such as silicon or indium gallium arsenide photodetectors, in several aspects.

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Spectroscopic photodetection plays a key role in many emerging applications such as context-aware optical sensing, wearable biometric monitoring, and biomedical imaging. Photodetectors based on organic semiconductors open many new possibilities in this field. However, ease of processing, tailorable optoelectronic properties, and sensitivity for faint light are still significant challenges.

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Early detection of malign patterns in patients' biological signals can save millions of lives. Despite the steady improvement of artificial intelligence-based techniques, the practical clinical application of these methods is mostly constrained to an offline evaluation of the patients' data. Previous studies have identified organic electrochemical devices as ideal candidates for biosignal monitoring.

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Persistent luminescence from triplet excitons in organic molecules is rare, as fast non-radiative deactivation typically dominates over radiative transitions. This work demonstrates that the substitution of a hydrogen atom in a derivative of phenanthroimidazole with an N-phenyl ring can substantially stabilize the excited state. This stabilization converts an organic material without phosphorescence emission into a molecular system exhibiting efficient and ultralong afterglow phosphorescence at room temperature.

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Detection of electromagnetic signals for applications such as health, product quality monitoring or astronomy requires highly responsive and wavelength selective devices. Photomultiplication-type organic photodetectors have been shown to achieve high quantum efficiencies mainly in the visible range. Much less research has been focused on realizing near-infrared narrowband devices.

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The success of metal halide perovskites in photovoltaic and light-emitting diodes (LEDs) motivates their application as a solid-state thin-film laser. Various perovskites have shown optically pumped stimulated emission of lasing and amplified spontaneous emission (ASE), yet the ultimate goal of electrically pumped stimulated emission has not been achieved. As an essential step toward this goal, here, a perovskite diode structure that simultaneously exhibits stable operation at high current density (≈1 kA cm ) and optically excited ASE (with a threshold of 180 µJ cm ) is reported.

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Blending organic molecules to tune their energy levels is currently being investigated as an approach to engineer the bulk and interfacial optoelectronic properties of organic semiconductors. It has been proven that the ionization energy and electron affinity can be equally shifted in the same direction by electrostatic effects controlled by blending similar halogenated derivatives with different energetics. Here we show that the energy gap of organic semiconductors can also be tuned by blending.

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Organic solar cells are approaching power conversion efficiencies of other thin-film technologies. However, in order to become truly market competitive, the still substantial voltage losses need to be reduced. Here, the synthesis and characterization of four novel arylamine-based push-pull molecular donors was described, two of them exhibiting a methyl group at the para-position of the external phenyl ring of the arylamine block.

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