Understanding the excitonic nature of excited states in two-dimensional (2D) transition-metal dichalcogenides (TMDCs) is of key importance to make use of their optical and charge transport properties in optoelectronic applications. We contribute to this by the direct experimental determination of the exciton binding energy (Eb,exc) of monolayer MoS2 and WSe2 on two fundamentally different substrates, i.e. the insulator sapphire and the metal gold. By combining angle-resolved direct and inverse photoelectron spectroscopy we measure the electronic band gap (Eg), and by reflectance measurements the optical excitonic band gap (Eexc). The difference of these two energies is Eb,exc. The values of Eg and Eb,exc are 2.11 eV and 240 meV for MoS2 on sapphire, and 1.89 eV and 240 meV for WSe2 on sapphire. On Au Eb,exc is decreased to 90 meV and 140 meV for MoS2 and WSe2, respectively. The significant Eb,exc reduction is primarily due to a reduction of Eg resulting from enhanced screening by the metal, while Eexc is barely decreased for the metal support. Energy level diagrams determined at the K-point of the 2D TMDCs Brillouin zone show that MoS2 has more p-type character on Au as compared to sapphire, while WSe2 appears close to intrinsic on both. These results demonstrate that the impact of the dielectric environment of 2D TMDCs is more pronounced for individual charge carriers than for a correlated electron–hole pair, i.e. the exciton. A proper dielectric surrounding design for such 2D semiconductors can therefore be used to facilitate superior optoelectronic device function.
An ion-sensitive electrolyte-gated organic field-effect transistor for selective and reversible detection of sodium (Na(+) ) down to 10(-6) M is presented. The inherent low voltage - high current operation of these transistors in combination with a state-of-the-art ion-selective membrane proves to be a novel, versatile modular sensor platform.
A unique implementation of an organic image detector using resistive photo-switchable pixels is presented. This resistive photo-switch comprises the vertical integration of an organic photodiode and an organic resistive switching memory element. The photodiodes act as a photosensitive element while the resistive switching elements simultaneously store the detected light information.
Molecular doping allows enhancement and precise control of electrical properties of organic semiconductors, and is thus of central technological relevance for organic (opto‐) electronics. Beyond single‐component molecular electron acceptors and donors, organic salts have recently emerged as a promising class of dopants. However, the pertinent fundamental understanding of doping mechanisms and doping capabilities is limited. Here, the unique capabilities of the salt consisting of a borinium cation (Mes2B+; Mes: mesitylene) and the tetrakis(penta‐fluorophenyl)borate anion [B(C6F5)4]− is demonstrated as p‐type dopant for polymer semiconductors. With a range of experimental methods, the doping mechanism is identified to comprise electron transfer from the polymer to Mes2B+, and the positive charge on the polymer is stabilized by [B(C6F5)4]−. Notably, the former salt cation leaves during processing and is not present in films. The anion [B(C6F5)4]− even enables the stabilization of polarons and bipolarons in poly(3‐hexylthiophene), not yet achieved with other molecular dopants. From doping studies with high ionization energy polymer semiconductors, the effective electron affinity of Mes2B+[B(C6F5)4]− is estimated to be an impressive 5.9 eV. This significantly extends the parameter space for doping of polymer semiconductors.
Inkjet printing (IJP) has evolved over the past 30 years into a reliable, versatile, and cost‐effective industrial production technology in many areas from graphics to printed electronic applications. Intensive research efforts have led to the successful development of functional electronic inks to realize printed circuit boards, sensors, lighting, actuators, energy storage, and power generation devices. Recently, a promising solution‐processable material class has entered the stage: metal halide perovskites (MHPs). Within just 10 years of research, the efficiency of perovskite solar cells (PSCs) on a laboratory scale increased to over 25%. Despite the complex nature of MHPs, significant progress has also been made in controlling film formation in terms of ink development, substrate wetting behavior, and crystallization processes of inkjet‐printed MHPs. This results in highly efficient inkjet‐printed PSCs with a power conversion efficiency (PCE) of almost 21%, paving the way for cost‐effective and highly efficient thin‐film solar cell technology. In addition, the excellent optoelectronic properties of inkjet‐printed MHPs achieve remarkable results in photodetectors, X‐ray detectors, and illumination applications. Herein, a comprehensive overview of the state‐of‐the‐art and recent advances in the production of inkjet‐printed MHPs for highly efficient and innovative optoelectronic devices is provided.
Van der Waals heterostructures consisting of 2D semiconductors and conjugated molecules are of increasing interest because of the prospect of a synergistic enhancement of (opto)electronic properties. In particular, perylenetetracarboxylic dianhydride (PTCDA) on monolayer (ML)‐MoS2 has been identified as promising candidate and a staggered type‐II energy level alignment and excited state interfacial charge transfer have been proposed. In contrast, it is here found with inverse and direct angle resolved photoelectron spectroscopy that PTCDA/ML‐MoS2 supported by insulating sapphire exhibits a straddling type‐I level alignment, with PTCDA having the wider energy gap. Photoluminescence (PL) and sub‐picosecond transient absorption measurements reveal that resonance energy transfer, i.e., electron–hole pair (exciton) transfer, from PTCDA to ML‐MoS2 occurs on a sub‐picosecond time scale. This gives rise to an enhanced PL yield from ML‐MoS2 in the heterostructure and an according overall modulation of the photoresponse. These results underpin the importance of a precise knowledge of the interfacial electronic structure in order to understand excited state dynamics and to devise reliable design strategies for optimized optoelectronic functionality in van der Waals heterostructures.
Monolayer (ML) transition metal dichalcogenides (TMDCs) are an attracting new class of two-dimensional direct band gap semiconducting materials for optoelectronic device applications. The combination of TMDCs with organic semiconductors holds the promise to further improve device properties with added functionality. Here we demonstrate that excited state charge transfer from a thin organic absorber layer, i.e. metal-free phthalocyanine (H 2 Pc), enhances the photoresponse of ML MoS 2 dramatically and at the same time also significantly extends it to spectral regions where the TMDC is transparent. The fundamental processes enabling this boost in photodetector performance are unraveled by a combination of photoemission (PES), photoluminescence (PL) and photocurrent action spectroscopy. Direct and inverse PES reveal a type II energy level alignment at the MoS 2 /H 2 Pc interface with a large energy offset of 1 eV, which is sufficient to drive the excited state charge transfer. Time-resolved PL measurements evidence highly efficient dissociation of excitons generated in H 2 Pc when they are in contact with MoS 2 . Exciton dissociation results in the formation of a charge-separated state at the hybrid interface with an energy gap of ca. 1.2 eV, in accordance with PES. This state then dissociates into free carriers and markedly contributes to the current in the photodetector, as demonstrated by photocurrent action spectroscopy. This reveals that the photoconductivity within the MoS 2 ML is generated by light directly absorbed in the TMDC and, notably, with comparable efficiency by the absorption of H 2 Pc. The present demonstration of highly efficient carrier generation in TMDC/organic hybrid structures paves the way for future nanoscale photodetectors with very wide spectral sensitivity.
A comprehensive understanding of the energy level alignment mechanisms between two-dimensional (2D) semiconductors and electrodes is currently lacking, but it is a prerequisite for tailoring the interface electronic properties to the requirements of device applications. Here, we use angle-resolved direct and inverse photoelectron spectroscopy to unravel the key factors that determine the level alignment at interfaces between a monolayer of the prototypical 2D semiconductor MoS2 and conductor, semiconductor, and insulator substrates. For substrate work function (Φsub) values below 4.5 eV we find that Fermi level pinning occurs, involving electron transfer to native MoS2 gap states below the conduction band. For Φsub above 4.5 eV, vacuum level alignment prevails but the charge injection barriers do not strictly follow the changes of Φsub as expected from the Schottky-Mott rule. Notably, even the trends of the injection barriers for holes and electrons are different. This is caused by the band gap renormalization of monolayer MoS2 by dielectric screening, which depends on the dielectric constant (εr) of the substrate. Based on these observations, we introduce an expanded Schottky-Mott rule that accounts for band gap renormalization by εr -dependent screening and show that it can accurately predict charge injection barriers for monolayer MoS2. It is proposed that the formalism of the expanded Schottky-Mott rule should be universally applicable for 2D semiconductors, provided that material-specific experimental benchmark data are available.
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