Only gold can pull this off: mechanical exfoliations of transition metal dichalcogenides beyond scotch tape

Following in graphene’s wake, the scotch tape method became the key enabler for the preparation of 2D materials, providing easy access to high-quality materials mainly limited by low yield. At this time, transition metal dichalcogenides (TMDC) received tremendous attention as a promising class of two-dimensional (2D) semiconductors. The motivation to reach the 2D limit of TMDCs and many other layered materials has long been set, and with the rise of gold-mediated exfoliations towards the millimeter scale, the stacking of these 2D single-layer building blocks into artificial 3D lattices is more relevant than ever. On this note, this review presents the recent developments in gold-mediated exfoliations beyond scotch tape, accompanied by a methods walkthrough for such a process. These matured gold exfoliations unlock a whole palette of 2D building blocks, ready for the assembly of macroscopic van der Waals heterostructures, or twistronics. Ultimately, mechanical exfoliation as a key enabler for high-quality single layers, evolved from scotch tape to gold, and became an even more potent tool in the process.Peer Reviewe

Gentle plasma process for embedded silver-nanowire flexible transparent electrodes on temperature-sensitive polymer substrates

The present study investigates processing routes to obtain highly conductive and transparent electrodes of silver nanowires (AgNWs) on flexible polyethylene terephthalate (PET) substrate. The AgNWs are embedded into a UV-curable polymer to reduce the electrode roughness and enhance its stability. For the purpose of device integration, the AgNWs must partially protrude from the polymer, which demands that their embedding is followed by a transfer step from a host substrate to the final substrate. Since the AgNWs require some sort of curing (thermal or plasma) to reduce the electrode sheet resistance, a thermally stable host substrate is generally used. This study shows that both thermally stable polyimide, as well as temperature-sensitive PET can be used as flexible host substrates, combined with a gentle, AgNW plasma curing. This is possible by adjusting the fabrication sequence to accommodate the plasma curing step, depending on the host substrate. As a result, embedded AgNW electrodes, transferred from polyimide-to-PET and from PET-to-PET are obtained, with optical transmittance of ∼80% (including the substrate) and sheet resistance of ∼13 Ω/sq., similar to electrodes transferred from glass-to-glass substrates. The embedded AgNW electrodes on PET show superior performance in bending tests, as compared to indium-tin-oxide electrodes. The introduced approach, involving low-cost flexible substrates, AgNW spray-coating and plasma curing, is compatible with high-throughput, roll-to-roll processing.Klima- und Energiefondshttp://dx.doi.org/10.13039/100008559Österreichische Forschungsförderungsgesellschafthttp://dx.doi.org/10.13039/501100004955Peer Reviewe

Binary Addressable Optical Multiplexing Waveguides via Electrochromic Switching

Photonic circuits attract much attention as promising candidates to overcome the drawbacks of their electronic counterparts. By utilizing the broad bandwidth and low energy consumption of optical communication, hybrid circuits can provide a comprehensive platform for the era beyond Moore's law. In particular, parallel matrix operations, the heavy lifting behind neural networks, remain challenging for traditional electronics due to high heat dissipation. To enable these parallel computations optically, (de-)multiplexing is crucial to address the different channels. Previously this has been accomplished with complex spectral or time encodings in wave division or time division methods. However, herein, a simple method to address parallel optical channels exclusively with 2-bit signals is presented. By using PEDOT:PSS as electrochromic material for intensity modulation, light transmission or absorption is controlled by oxidation and reduction with an electrolyte. Y-branch structures are used to design the multiplexing layout and to assign the 2-bit states to the channels. This binary addressable optical multiplexer, therefore, combines optical communication with electronic signals into a hybrid circuit.Peer Reviewe

Exciton and Excited-State Charge Transfer at 2D van der Waals Interfaces

Combining materials with diverse properties into two‐dimensional (2D) van der Waals heterostructures lies at the heart of electronic, optoelectronic, and photonic applications. Prerequisite is a significant degree of electronic or photonic coupling of the constituents across the heterointerface. Understanding and controlling these interactions is mandatory to achieve the desired functionality. This review focuses on the charge and energy transfer processes and their dynamics in a specific class of van der Waals heterostructures, namely such composed of semiconducting transition metal dichalcogenides and conjugated organic molecules. With the help of prototypical material combinations, the importance of a precise knowledge of the interfacial electronic structure is demonstrated as it governs the excited‐state dynamics. This review aims at providing basic design guidelines to achieve functional 2D organic/inorganic van der Waals heterostructures with final properties that can be designed by careful selection of the organic component.Peer Reviewe

Multipitched plasmonic nanoparticle grating for broadband light enhancement in white light‑emitting organic diodes

We apply regular arrays of plasmonic nanodisks to enhance light emission from an organic white light-emitting diode (WOLED). To achieve broadband enhancement, we apply, first, aluminum as a nanodisk material with moderate loss throughout the whole visible spectral range. Second, broadband light coupling is mediated by surface lattice resonances from a multipitch array built from two superimposed gratings with different grating constants formed by elliptic and circular nanodisks. To demonstrate the viability of this concept, the grating structure was embedded in the hole transport layer of a solution-processed phosphorescent WOLED exhibiting a current efficiency of 2.1 cd/A at 1000 cd/m2. The surface lattice resonances in the grating raise the current efficiency of the device by 23% to 2.6 cd/A at 1000 cd/m2, while the device emission changes from a neutral white to a warm white appearance with CIE1931 (x,y) coordinates of (0.361, 0.352) and (0.404, 0.351), respectively. The WOLED was characterized in detail optically by extinction and angle-resolved photoluminescence and as well by electroluminescence measurements for its opto-electronic characteristics. The experimental results agree well with finite-difference time domain simulations that aim at a better understanding of the underlying physical mechanisms. In summary, our work presents a novel versatile approach for achieving broadband enhancement of light emission in WOLEDs over a wide spectral range.Peer Reviewe

Large area inkjet-printed metal halide perovskite LEDs enabled by gas flow assisted drying and crystallization

We demonstrate the upscaling of inkjet-printed metal halide perovskite light-emitting diodes. To achieve this, the drying process, critical for controlling the crystallization of the perovskite layer, was optimized with an airblade-like slit nozzle in a gas flow assisted vacuum drying step. This yields large, continuous perovskite layers in light-emitting diodes with an active area up to 1600 mm2.Peer Reviewe

Resonance Energy Transfer from Monolayer WS2 to Organic Dye Molecules: Conversion of Faint Visible-Red into Bright Near-Infrared Luminescence

The synergetic combination of transition metal dichalcogenides (TMDCs) with organic dye molecules in functional heterostructures is promising for various optoelectronic applications. Here resonance energy transfer (RET) from a red‐emitting WS2 monolayer (1L‐WS2) to a layer of near‐infrared (NIR) emitting organic dye molecules is demonstrated. It is found that the total photoluminescence (PL) yield of the heterostructures is up to a factor of eight higher as compared to the PL yield of pristine 1L‐WS2. This is attributed to the efficient conversion of the mostly non‐radiative excitons in 1L‐WS2 into radiative excitons in the dye layer. A type‐I energy level alignment of the 1L‐WS2/dye interface assures the emission of bright PL. From excitation density‐dependent PL experiments, it is concluded that RET prevails against defect‐assisted non‐radiative recombination as well as Auger‐type exciton‐exciton annihilation in 1L‐WS2. The work paves the way for employing organic dye molecules in heterostructures with TMDCs in nanoscale light‐emitting devices with improved efficiency and tunable color.Peer Reviewe

The Electronic Properties of a 2D Ruddlesden‐Popper Perovskite and its Energy Level Alignment with a 3D Perovskite Enable Interfacial Energy Transfer

The success of using 2D Ruddlesden-Popper metal halide perovskites (MHPs) in optoelectronic devices has ignited great interest as means for energy level tuning at the interface with 3D MHPs. Inter alia, the application of 2D phenylethylammonium lead quaternary iodide (PEA2PbI4)/3D MHPs interfaces has improved various optoelectronic devices, where a staggered type-II energy level alignment is often assumed. However, a type-II heterojunction seems to contradict the enhanced photoluminescence observed for 2D PEA2PbI4/3D MHP interfaces, which raises fundamental questions about the electronic properties of such junctions. In this study, using direct and inverse photoelectron spectroscopy, it is revealed that a straddling type-I energy level alignment is present at 2D PEA2PbI4/3D methylammonium lead triiodide (MAPbI3) interfaces, thus explaining that the photoluminescence enhancement of the 3D perovskite is induced by energy transfer from the 2D perovskite. These results provide a reliable fundamental understanding of the electronic properties at the investigated 2D/3D MHP interfaces and suggest careful (re)consideration of the electronic properties of other 2D/3D MHP heterostructures.Peer Reviewe

The impact of plasmonic electrodes on the photocarrier extraction of inverted organic bulk heterojunction solar cells

Nano-patterning the semiconducting photoactive layer/back electrode interface of organic photovoltaic devices is a widely accepted approach to enhance the power conversion efficiency through the exploitation of numerous photonic and plasmonic effects. Yet, nano-patterning the semiconductor/metal interface leads to intertwined effects that impact the optical as well as the electrical characteristic of solar cells. In this work we aim to disentangle the optical and electrical effects of a nano-structured semiconductor/metal interface on the device performance. For this, we use an inverted bulk heterojunction P3HT:PCBM solar cell structure, where the nano-patterned photoactive layer/back electrode interface is realized by patterning the active layer with sinusoidal grating profiles bearing a periodicity of 300 nm or 400 nm through imprint lithography while varying the photoactive layer thickness (LPAL) between 90 and 400 nm. The optical and electrical device characteristics of nano-patterned solar cells are compared to the characteristics of control devices, featuring a planar photoactive layer/back electrode interface. We find that patterned solar cells show for an enhanced photocurrent generation for a LPAL above 284 nm, which is not observed when using thinner active layer thicknesses. Simulating the optical characteristic of planar and patterned devices through a finite-difference time-domain approach proves for an increased light absorption in presence of a patterned electrode interface, originating from the excitation of propagating surface plasmon and dielectric waveguide modes. Evaluation of the external quantum efficiency characteristic and the voltage dependent charge extraction characteristics of fabricated planar and patterned solar cells reveals, however, that the increased photocurrents of patterned devices do not stem from an optical enhancement but from an improved charge carrier extraction efficiency in the space charge limited extraction regime. Presented findings clearly demonstrate that the improved charge extraction efficiency of patterned solar cells is linked to the periodic surface corrugation of the (back) electrode interface.Peer Reviewe

A guide to qualitative haze measurements demonstrated on inkjet-printed silver electrodes for flexible OLEDs

The search for alternative transparent electrodes to the commonly used indium tin oxide (ITO) in optoelectronic devices has led to solution-based approaches based on inkjet printing. As an additive manufacturing technique that allows drops to be positioned only where necessary, inkjet printing shows reduced waste of starting material compared to other methods such as spin coating. As a result, functional materials can be both coated and structured without the need for masks or lithographic pre-patterning of the substrate. For this contribution, we utilized a particle-free silver ink to produce a transparent electrode by inkjet printing. After printing, the silver ions were reduced to metallic silver by an argon plasma. The process takes place at low temperatures (ca. 40 – 50°C), making it suitable for use with flexible substrates, which are often temperature-sensitive. The printed silver layers show good electrical conductivity and optical transmittance, with a crystalline grain structure being formed and maintained during the metallization process. This structure forms a self-organized nanometer-size grid, whose structure allows light to pass through. Due to its nano-structured property, the haze of the electrode was investigated using a simple experimental setup based on a light source shining through the electrode and analyzing the size of the projected pattern. Such qualitative assessment can be a useful indication of the quality of the electrode and we provide details on how to replicate this setup. The final electrodes were implemented in solution-processed OLEDs, which showed bright luminance and overall low haze compared to ITO-based reference devices.Peer Reviewe