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Sebastian Reineke

Publications and source records attributed to Sebastian Reineke.

18 recordsLinked to original sources

Round-Robin Test of a Light-Emitting Electrochemical Cell: Establishing a Reference Protocol for Quality Research

Emerging technologies benefit from a jointly established reference protocol, which can lower the bar of entry for new researchers while serving as a calibration standard for established actors. The light-emitting electrochemical cell (LEC) combines electrochemistry and optoelectronics in an intricate manner, and it can by that enable sustainable and commercially relevant printing fabrication of emissive thin-film devices. However, LEC performance is sensitive to a range of material and processing parameters, which frequently results in inadequate, or even erroneous, device evaluation. With this in mind, we present herein a LEC reference protocol, which details the sourcing of materials and the procedures and parameters for robust device fabrication and operation. The protocol has been tested across nine international research groups, and the collected results from this interlaboratory round-robin test confirm that good LEC performance can be reproducibly obtained following our protocol. We also identify common pitfalls that can arise during LEC development, and present practical steps for attaining optimum LEC performance. We hope this reference protocol will improve the quality of future LEC research and serve as a guide for future researchers entering this vibrant field.

cond-mat.soft

Efficient purely organic phosphorescent emitters for programmable luminescent tags: from building blocks to donor-acceptor-donor structures

Purely organic room-temperature phosphorescence (RTP) emitters are key components of programmable luminescent tags (PLTs), photonic devices for rewritable information storage and UV dosimetry. In this work, we systematically explore the design space of donor-acceptor and donor-acceptor-donor organic phosphorescent emitters in symmetric and asymmetric architectures. Phenoxathiine (PX) is introduced as an alternative donor to thianthrene (TA), combined with benzophenone (BP) or pyridine (Py) as acceptors. Through photophysical characterization, quantum chemical simulations, and PLT device testing, we identify structure-property relationships and, in particular, investigate the impact of the individual moieties on the emission properties and stability. The RTP emission wavelength is primarily tunable through the donor moiety: PX-based emitters emit sky-blue ({\lambda}_P = 480 nm), while TA-based emitters emit in the green ({\lambda}_P = 520 nm) due to an increased Stokes shift. The acceptor unit strongly influences the phosphorescence quantum yield, with Py-based emitters systematically outperforming BP-based ones. All newly synthesized PX-containing emitters show sufficient performance in PLT devices, though with reduced photostability compared to TA-based counterparts. Together, these results demonstrate that systematic donor-acceptor design enables predictable control over RTP emission properties, advancing the rational development of high-performance RTP-based photonic devices.

cond-mat.mtrl-sci

High-Efficiency Deep Blue Single-Gaussian Europium(II) Emitters and their Emitter-Host Interactions

Eu(II) complexes are attractive emitters for deep-blue organic light-emitting diodes (OLEDs) due to their narrow, parity-allowed 4f-5d emission; however, their implementation in vacuum-processed OLEDs has remained limited. Here, we introduce a new molecular design concept for Eu(II) emitters, in which a crown-ether ligand is combined with carborate anions to define the coordination environment and improve steric shielding of the europium center. Based on this design, we present two emitters that combine narrow deep-blue photoluminescence with quantum yields approaching 90% and sufficient thermal stability for vacuum deposition. As the excited state dynamics of this emitter class are different from most conventional OLED emitters and the pathway to maximum luminescence efficiency in thin films is not fully established, we study interactions between Eu(II) complexes and the host environment, based on density functional theory and time-resolved experiments. We identify steric shielding of the Eu(II) core and energetic confinement of the excited 5d electron, defined by molecular design as key factors governing efficient luminescence, providing a roadmap for rational design of Eu(II) emitters. Together, these results establish a basis for higher-efficiency and deeper blue OLEDs incorporating Eu(II) emitters.

physics.app-ph

Blue Organic Light-Emitting Diodes with External Quantum Efficiencies over 20% Based on Europium(II) Emitters

The realization of blue electroluminescence with high efficiency and lifetime remains a long-standing hurdle for organic light-emitting diode (OLED) technology to overcome. Divalent Europium [Europium(II)] complexes offer a fundamentally distinct pathway toward this goal, as their atomic 4f-5d transitions yield single-Gaussian, spectrally pure emission with theoretical 100% exciton utilization in electroluminescence and no involvement of fragile organic bonds in the emissive process. Here, we present a rigid aza-crown europium(II) complex (Eu5NHCrown) that achieves near-unity photoluminescence quantum yield with bright, pure-blue emission and its incorporation in OLEDs. The emitter complex sublimes without decomposition and can be processed by industry-standard vacuum deposition. A bottom-emitting, single-host OLED architecture delivers an external quantum efficiency (EQE) of 20.7% with minimal roll-off (19.3% at 1000 cd m${}^{-2}$ ) and a narrowband electroluminescence with Commission Internationale de l'Eclairage (CIE) coordinates of (0.12, 0.25). This ligand design provides enhanced steric shielding of the Eu(II) center, enabling the highest reported efficiency among vacuum-deposited Eu(II)- based blue OLEDs while maintaining performance at high luminance. These results reveal the true potential of divalent Europium 4f-5d transitions for high-efficiency blue OLEDs, establishing a molecular design concept that bridges atomic-transition efficiency with the processability of organic materials.

physics.app-ph

Analysis of the Annealing Budget of Metal Oxide Thin-Film Transistors Prepared by an Aqueous Blade-Coating Process

Metal oxide (MO) semiconductors are widely used in electronic devices due to their high optical transmittance and promising electrical performance. This work describes the advancement toward an eco-friendly, streamlined method for preparing thin-film transistors (TFTs) via a pure water-solution blade-coating process with focus on a low thermal budget. Low temperature and rapid annealing of triple-coated indium oxide thin-film transistors (3C-TFTs) and indium oxide/zinc oxide/indium oxide thin-film transistors (IZI-TFTs) on a 300 nm SiO2 gate dielectric at 300 $^{\circ}$C for only 60 s yields devices with an average field effect mobility of 10.7 and 13.8 cm2/Vs, respectively. The devices show an excellent on/off ratio (>10^6), and a threshold voltage close to 0 V when measured in air. Flexible MO-TFTs on polyimide substrates with AlOx dielectrics fabricated by rapid annealing treatment can achieve a remarkable mobility of over 10 cm2/Vs at low operating voltage. When using a longer post-coating annealing period of 20 min, high-performance 3C-TFTs (over 18 cm2/Vs) and IZI-TFTs (over 38 cm2/Vs) using MO semiconductor layers annealed at 300 $^{\circ}$C are achieved.

physics.app-ph

Interdot Lead Halide Excess Management in PbS Quantum Dot Solar Cells

Light-harvesting devices made from PbS quantum dot (QD) absorbers are one of the many promising technologies of third-generation photovoltaics. Their simple, solution-based fabrication together with a highly tunable and broad light absorption makes their application in newly developed solar cells particularly promising. In order to yield devices with reduced voltage and current losses, PbS QDs need to have strategically passivated surfaces, most commonly achieved through lead iodide and bromide passivation. The interdot spacing is then predominantly filled with residual amorphous lead halide species that remain from the ligand exchange, thus hindering efficient charge transport and reducing device stability. Herein, we demonstrate that a post-treatment by iodide based 2-phenylethlyammonium salts (X-PEAI) and intermediate 2D perovskite formation can be used to manage the lead halide excess in the PbS QD active layer. This treatment results in improved device performance and increased shelf-life stability, demonstrating the importance of interdot spacing management in PbS quantum dot photovoltaics.

physics.app-ph

Structural order promotes efficient separation of delocalized charges at molecular heterojunctions

The energetic landscape at the interface between electron donating and accepting molecular materials favors efficient conversion of intermolecular charge-transfer states (CTS) into free charge carriers in high-performance organic solar cells. Here, we elucidate how interfacial energetics, charge generation and radiative recombination are affected by structural ordering. We experimentally determine the CTS binding energy of a series of model, small molecule donor-acceptor blends, where the used acceptors (B2PYMPM, B3PYMPM and B4PYMPM) differ only in the nitrogen position of their lateral pyridine rings. We find that the formation of an ordered, face-on molecular packing in B4PYMPM is beneficial to efficient, field-independent charge separation, leading to fill factors over 70% in photovoltaic devices. This is rationalized by a comprehensive computational protocol showing that, compared to the more amorphous and isotropically oriented B2PYMPM, the higher order of the B4PYMPM molecules provides more delocalized CTS. Furthermore, we find no correlation between the quantum efficiency of radiative free charge carrier recombination and the bound or unbound nature of the CTS. This work highlights the importance of structural ordering at donor-acceptor interfaces for efficient free carrier generation and shows that more ordering and less bound CT states do not preclude efficient radiative recombination.

physics.app-ph

Accurate wavelength tracking by exciton spin mixing

Wavelength discriminating systems typically consist of heavy benchtop-based instruments, comprising diffractive optics, moving parts, and adjacent detectors. For simple wavelengths 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, light-weight, easy-to-process, and flexible single-pixel devices are attracting increasing attention. Here, we propose a device for wavelength tracking with room-temperature phosphorescence at the heart of its functionality that demonstrates a resolution down to one nanometer and below. It is solution-processed from a single host-guest system comprising organic room-temperature phosphors and colloidal quantum dots. The share of excited triplet states within the photoluminescent layer is dependent on the excitation wavelength and determines the afterglow intensity of the film, which is tracked by a simple photodetector. Finally, an all-organic thin-film wavelength sensor and two applications are demonstrated where our novel measurement concept successfully replaces a full spectrometer.

physics.optics

A simple strategy to measure the contact resistance between metals and doped organic films

Charge injection from electrodes into doped organic films is a widespread technology used in the majority of state-of-the-art organic semiconductor devices. Although such interfaces are commonly considered to form Ohmic contacts via strong band bending, an experiment that directly measures the contact resistance has not yet been demonstrated. In this study, we use a simple metal/doped organic semiconductor/metal stack and study its voltage-dependent resistance. A transport layer thickness variation proves that the presented experiment gains direct access to the contact resistance of the device. We can quantify that for an operating current density of 10mA/cm2 the investigated material system exhibits a voltage drop over the metal/organic interface of about 200mV, which can be reduced by more than one order of magnitude when employing an additional injection layer. The presented experiment proposes a simple strategy to measure the contact resistance between any metal and doped organic film without applying numerical tools or elaborate techniques. Furthermore, the simplistic device architecture allows for very high, homogeneous, and tunable electric fields within the organic layer, which enables a clear investigation of the Poole-Frenkel effect.

physics.app-ph

High-speed and continuous-wave programmable luminescent tags

Most materials recently developed for room temperature phosphorescence (RTP) lack of practical relevance due to their inconvenient crystalline morphology. Using amorphous material systems instead, programmable luminescent tags (PLTs) based on organic biluminescent emitter molecules with easy processing and smooth sample shapes were presented recently. Here, the effective quenching of the emitters RTP by molecular oxygen (O2) and the consumption of the excited singlet O2 through a chemical reaction represent the central features. With customized activation schemes, high resolution content can be written and later erased multiple times into such films, providing a versatile yet simple photonic platform for information storage. However, two important limitations remain: (i) The immutable fluorescence of the emitters outshines the phosphorescent patterns by roughly one order of magnitude, allowing read-out of the PLTs only after the excitation source is turned off. (ii) The programming of these systems is a rather slow process, where lowest reported activation times are still > 8 s. Here, a material-focused approach to PLTs with fast activation times of 120 +/- 20 ms and high-contrast under continuous-wave (cw) illumination is demonstrated, leading to accelerated programming on industry relevant time scales and a simplified readout process both by eye and low cost cameras.

physics.app-ph

Parameter Optimization of Light Outcoupling Structures for High-Efficiency Organic Light-Emitting Diodes

Organic light-emitting diodes (OLEDs) have successfully entered the display market and continue to be attractive for many other applications. As state-of-the-art OLEDs can reach an internal quantum efficiency (IQE) of almost 100 %, light outcoupling remains one of the major screws left to be turned. The fact that no superior outcoupling structure has been found underlines that further investigations are needed to understand their prospect. In this paper, we use two-dimensional titanium dioxide (2D TiO$_2$) block arrays as a model of an internal light outcoupling structure and investigate the influence of its geometrical parameters on achieving the highest external quantum efficiency (EQE) for OLEDs. The multivariable problem is evaluated with the visual assistance of scatter plots, which enables us to propose an optimal period range and block width-to-distance ratio. The highest EQE achieved is 45.2 % with internal and external structures. This work contributes to the highly desired prediction of ideal light outcoupling structures in the future.

physics.app-ph

Organic Light-Emitting Diode Beam Shaping: Pixel Design for Variable Angular Emission Profile Control

Organic light-emitting diodes (OLEDs) are the leading self-emitting pixel technology in current and future small and large area displays. Once integrated with a certain layer architecture into the backplane layout, their emission colour and angular distribution is set by the optical properties of the layered system. In this paper, we demonstrate a pixel design that allows for actively controlled variation of the angular emission profile of the individual vertical pixel. For this, a tandem device is developed that comprises two units optimized for different angular emission pattern. We constrained the system to operate in a narrow emission band to maintain monochromaticity of the individual pixel. We discuss this concept for a red phosphorescence-based OLED stack and give an outlook based on simulations for the other primary display colours green and blue. The tandem unit can be operated with only two electrodes making use of the AC/DC driving concept, where the outer electrodes are in direct connection. In this paper, we will discuss the potential, status, and technology challenges for this concept.

physics.app-ph

Interplay of Fluorescence and Phosphorescence in Organic Biluminescent Emitters

Biluminescent organic emitters show simultaneous fluorescence and phosphorescence at room temperature. So far, the optimization of the room temperature phosphorescence (RTP) in these materials has drawn the attention of research. However, the continuous wave operation of these emitters will consequently turn them into systems with vastly imbalanced singlet and triplet populations, which is due to the respective excited state lifetimes. This study reports on the exciton dynamics of the biluminophore NPB (N,N-di(1-naphthyl)-N,N-diphenyl-(1,1-biphenyl)-4,4-diamine). In the extreme case, the singlet and triplet exciton lifetimes stretch from 3 ns to 300 ms, respectively. Through sample engineering and oxygen quenching experiments, the triplet exciton density can be controlled over several orders of magnitude allowing to studying exciton interactions between singlet and triplet manifolds. The results show, that singlet-triplet annihilation reduces the overall biluminescence efficiency already at moderate excitation levels. Additionally, the presented system represents an illustrative role model to study excitonic effects in organic materials.

physics.chem-ph

Real-time beam-shaping without additional optical elements

Providing artificial light and enhancing the quality of the respective light sources is of continued interest in the fields of solid state-, condensed matter, and semiconductor physics. A lot of research has been done to increase luminous efficiency, lifetime and colour stability of such devices. However, the emission characteristics of a given light source don't necessarily comply with today's, often sophisticated applications. Here, beam-shaping deals with the transformation of a given light distribution into a customized one. This is achieved by secondary optical elements often sporting elaborate designs, where the actual light source takes up only a small fraction of the system's volume. Such designs limit the final light source to one permanent operation mode, which can only be overcome by employing mechanically-adjustable optical elements. Here, we show that organic light-emitting diodes (OLEDs) make real-time regulation of a beam-shape possible, without relying on secondary optical elements and without using any mechanical adjustment. For a red light-emitting two-unit OLED architecture, we demonstrate the ability of continuous tuning between strongly forward and strongly sideward emission, where the device efficiency is maintained at an application relevant level ranging between 6-8% external quantum efficiency (EQE) for any setting chosen. In combination with additional optical elements, customizable and tunable systems are possible, whereby the tuning stems from the light source itself rather than from the secondary optics.

physics.optics

Enhanced light emission from top-emitting organic light-emitting diodes by optimizing surface plasmon polariton losses

We demonstrate enhanced light extraction for monochrome top-emitting organic light-emitting diodes (OLEDs). The enhancement by a factor of 1.2 compared to a reference sample is caused by the use of a hole transport layer (HTL) material possessing a low refractive index (1.52). The low refractive index reduces the in-plane wave vector of the surface plasmon polariton (SPP) excited at the interface between the bottom opaque metallic electrode (anode) and the HTL. The shift of the SPP dispersion relation decreases the power dissipated into lost evanescent excitations and thus increases the outcoupling efficiency, although the SPP remains constant in intensity. The proposed method is suitable for emitter materials owning isotropic orientation of the transition dipole moments as well as anisotropic, preferentially horizontal orientation, resulting in comparable enhancement factors. Furthermore, for sufficiently low refractive indices of the HTL material, the SPP can be modeled as a propagating plane wave within other organic materials in the optical microcavity. Thus, by applying further extraction methods, such as micro lenses or Bragg gratings, it would become feasible to obtain even higher enhancements of the light extraction.

physics.optics

Room temperature triplet state spectroscopy of organic semiconductors

Organic light emitting devices and solar cells are machines that create, manipulate and destroy excited states in organic semiconductors. It is crucial to characterize these excited states, or excitons, to optimize device performance in applications like displays and solar energy harvesting. This is complicated if the excited state is a triplet because the electronic transition is dark with a vanishing oscillator strength. As a consequence, triplet state spectroscopy must usually be performed at cryogenic temperatures to reduce competition from non-radiative rates. Here, we control non-radiative rates by engineering a solid-state host matrix containing the target molecule, allowing the observation of phosphorescence at room temperature and alleviating constraints of cryogenic experiments. We test these techniques on a wide range of materials with functionalities spanning multi-exciton generation (singlet exciton fission), organic light emitting device host materials, and thermally activated delayed fluorescence type emitters. Control of non-radiative modes in the matrix surrounding a target molecule may also have broader applications in light emitting and photovoltaic devices.

cond-mat.mtrl-sci

Highly efficient, dual state emission from an organic semiconductor

We report highly efficient, simultaneous fluorescence and phosphorescence (74% yield) at room temperature from a single molecule ensemble of (BzP)PB dispersed into a polymer host. The slow phosphorescence (208 ms lifetime) is very efficient (50%) at room temperature and only possible because the non-radiative rate for the triplet state is extremely low. The ability of an organic molecule to function as an efficient dual state emitter at room temperature is unusual and opens new fields of applications including the use as broadband down-conversion emitters, optical sensors and attenuators, exciton probes, and spin-independent intermediates for Förster resonant energy transfer.

cond-mat.mtrl-sci

White organic light-emitting diodes: Status and perspective

White organic light-emitting diodes (OLEDs) are ultra-thin, large-area light sources made from organic semiconductor materials. Over the last decades, much research has been spent on finding the suitable materials to realize highly efficient monochrome and white OLEDs. With their high efficiency, color-tunability, and color-quality, white OLEDs are emerging to become one of the next generation light sources. In this review, we discuss the physics of a variety of device concepts that are introduced to realize white OLEDs based on both polymer and small molecule organic materi als. Owing to the fact that about 80 % of the internally generated photons are trapped within the thin-film layer structure, we put a second focus on reviewing promising concepts for improved light outcoupling.

cond-mat.mtrl-sci