Routes for efficiency enhancement in fluorescent TADF exciplex host OLEDs gained from an electro‐optical device model

Fluorescence-based organic light-emitting diodes (OLEDs) using thermally activated delayed fluorescence (TADF) have increasingly attracted attention in research and industry. One method to implement TADF is based on an emitter layer composed of an exciplex host and a fluorescent dopant. Even though the experimental realization of this concept has demonstrated promising external quantum efficiencies, the full potential of this approach has not yet been assessed. To this end, a comprehensive electro-optical device model accounting for the full exciton dynamics including triplet harvesting and exciton quenching is presented. The model parameters are fitted to multiple output characteristics of an OLED comprising a TADF exciplex host with a fluorescent emitter, showing an external quantum efficiency of >10%. With the model at hand, an emission zone analysis and a parameter study are performed, and possible routes for further efficiency enhancement are presented

Density of bulk trap states in organic semiconductor crystals: discrete levels induced by oxygen in rubrene

The density of trap states in the bandgap of semiconducting organic single crystals has been measured quantitatively and with high energy resolution by means of the experimental method of temperature-dependent space-charge-limited-current spectroscopy (TD-SCLC). This spectroscopy has been applied to study bulk rubrene single crystals, which are shown by this technique to be of high chemical and structural quality. A density of deep trap states as low as ~ 10^{15} cm^{-3} is measured in the purest crystals, and the exponentially varying shallow trap density near the band edge could be identified (1 decade in the density of states per ~25 meV). Furthermore, we have induced and spectroscopically identified an oxygen related sharp hole bulk trap state at 0.27 eV above the valence band.Comment: published in Phys. Rev. B, high quality figures: http://www.cpfs.mpg.de/~krellner

Field-induced charge transport at the surface of pentacene single crystals: a method to study charge dynamics of 2D electron systems in organic crystals

A method has been developed to inject mobile charges at the surface of organic molecular crystals, and the DC transport of field-induced holes has been measured at the surface of pentacene single crystals. To minimize damage to the soft and fragile surface, the crystals are attached to a pre-fabricated substrate which incorporates a gate dielectric (SiO_2) and four probe pads. The surface mobility of the pentacene crystals ranges from 0.1 to 0.5 cm^2/Vs and is nearly temperature-independent above ~150 K, while it becomes thermally activated at lower temperatures when the induced charges become localized. Ruling out the influence of electric contacts and crystal grain boundaries, the results contribute to the microscopic understanding of trapping and detrapping mechanisms in organic molecular crystals.Comment: 14 pages, 4 figures. Submitted to J. Appl. Phy

Hole mobility in organic single crystals measured by a "flip-crystal" field-effect technique

We report on single crystal high mobility organic field-effect transistors (OFETs) prepared on prefabricated substrates using a "flip-crystal" approach. This method minimizes crystal handling and avoids direct processing of the crystal that may degrade the FET electrical characteristics. A chemical treatment process for the substrate ensures a reproducible device quality. With limited purification of the starting materials, hole mobilities of 10.7, 1.3, and 1.4 cm^2/Vs have been measured on rubrene, tetracene, and pentacene single crystals, respectively. Four-terminal measurements allow for the extraction of the "intrinsic" transistor channel resistance and the parasitic series contact resistances. The technique employed in this study shows potential as a general method for studying charge transport in field-accumulated carrier channels near the surface of organic single crystals.Comment: 26 pages, 7 figure

Unusually large enhancement of thermopower in an electric field induced two-dimensional electron gas

Two-dimensionally confined electrons showing unusually large thermopower (S) have attracted attention as a potential approach for developing high performance thermoelectric materials. However, enhanced S has never been observed in electric field induced two-dimensional electron gas (2DEG). Here we demonstrate electric field modulation of S for a field effect transistor (FET) fabricated on a SrTiO3 crystal using a water-infiltrated nanoporous glass as the gate insulator. An electric field application confined carrier electrons up to ~2E15 /cm^2 in an extremely thin (~2 nm) 2DEG. Unusually large enhancement of |S| was observed when the sheet carrier concentration exceeded 2.5E14 /cm^2, and it modulated from ~600 (~2E15 /cm^2) to ~950 {\mu}V/K (~8E14 /cm^2), which were approximately five times larger than those of the bulk, clearly demonstrating that an electric field induced 2DEG provides unusually large enhancement of |S|.Comment: 20 pages including 4 figures and Supporting Information, Advanced Materials (in press

UV/Ozone treatment to reduce metal-graphene contact resistance

We report reduced contact resistance of single-layer graphene devices by using ultraviolet ozone (UVO) treatment to modify the metal/graphene contact interface. The devices were fabricated from mechanically transferred, chemical vapor deposition (CVD) grown, single layer graphene. UVO treatment of graphene in the contact regions as defined by photolithography and prior to metal deposition was found to reduce interface contamination originating from incomplete removal of poly(methyl methacrylate) (PMMA) and photoresist. Our control experiment shows that exposure times up to 10 minutes did not introduce significant disorder in the graphene as characterized by Raman spectroscopy. By using the described approach, contact resistance of less than 200 {\Omega} {\mu}m was achieved, while not significantly altering the electrical properties of the graphene channel region of devices.Comment: 17 pages, 5 figure

DNA looping by FokI: the impact of twisting and bending rigidity on protein-induced looping dynamics

Protein-induced DNA looping is crucial for many genetic processes such as transcription, gene regulation and DNA replication. Here, we use tethered-particle motion to examine the impact of DNA bending and twisting rigidity on loop capture and release, using the restriction endonuclease FokI as a test system. To cleave DNA efficiently, FokI bridges two copies of an asymmetric sequence, invariably aligning the sites in parallel. On account of the fixed alignment, the topology of the DNA loop is set by the orientation of the sites along the DNA. We show that both the separation of the FokI sites and their orientation, altering, respectively, the twisting and the bending of the DNA needed to juxtapose the sites, have profound effects on the dynamics of the looping interaction. Surprisingly, the presence of a nick within the loop does not affect the observed rigidity of the DNA. In contrast, the introduction of a 4-nt gap fully relaxes all of the torque present in the system but does not necessarily enhance loop stability. FokI therefore employs torque to stabilise its DNA-looping interaction by acting as a ‘torsional’ catch bond

Measuring frontier orbital energy levels of OLED materials using cyclic voltammetry in solution

The operation of organic light emitting diodes (OLEDs) is governed by a range of material parameters, such as frontier orbital energy levels, charge carrier mobility and excitonic rate parameters. In state-of-the art numerical simulations of OLED devices, more than 30 parameters must be considered to describe the behavior of a multilayer device. Independent measurement techniques to reliably determine each material parameter individually are therefore highly desirable. While several techniques have been established in the OLED community to determine some of them, the highest occupied and lowest unoccupied molecular orbital (HOMO and LUMO) energy levels are not measured or reported on a regular basis, despite their significant influence on device performance. In this work, we show how cyclic voltammetry in solution can be used as a simple technique to measure the HOMO and LUMO energy levels of organic semiconductors. This easily performed experiment allows a fairly accurate estimation of the energy levels of the layers in a device stack. Cyclic voltammetry measurements of four typical OLED materials in solution are presented and their analysis is described in detail to encourage more such measurements in future OLED studies. Four distinctly different voltammograms were obtained, ranging from relatively ideal reversible behavior to a very non-ideal behavior, lacking electrochemical reverse reactions. Two methods for extracting the HOMO and LUMO energy levels from cyclic voltammetry are discussed and compared. The measured HOMO and LUMO levels compare well with reported values measured on thin films, showing that cyclic voltammetry in solution provides a viable means to determine this important, yet underinvestigated material property

Simulations, measurements and optimization of OLEDs with scattering layer

A multi-scale optical model for organic light-emitting devices containing scattering layers is presented. This model describes the radiation of embedded oscillating dipoles and scattering from spherical particles. After successful model validation with experiments on a top-emitting white OLED, we show how this tool can be used for optimization with specific targets