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Organic Light-Emitting Diodes Based on Conjugation-Induced Thermally Activated Delayed Fluorescence Polymers: Interplay Between Intra- and Intermolecular Charge Transfer States
In this work, interactions between different host materials and a blue TADF polymer named P1 are systematically investigated. In photoluminescence, the host can have substantial impact on the photoluminescence quantum yield (PLQY) and the intensity of delayed fluorescence (ΦDF), where more than three orders of magnitude difference of ΦDF in various hosts is observed, resulting from a polarity effect of the host material and energy transfer. Additionally, an intermolecular charge-transfer (CT) emission with pronounced TADF characteristics is observed between P1 and 2,4,6-tris[3-(diphenylphosphinyl)phenyl]-1,3,5-triazine (PO-T2T), with a singlet-triplet splitting of 7 meV. It is noted that the contribution of harvested triplets in monochrome organic light-emitting diodes (OLEDs) correlates with ΦDF. For devices based on intermolecular CT-emission, the harvested triplets contribute ~90% to the internal quantum efficiency. The results demonstrate the vital importance of host materials on improving the PLQY and sensitizing ΦDF of TADF polymers for efficient devices. Solution-processed polychrome OLEDs with a color close to a white emission are presented, with the emission of intramolecular (P1) and intermolecular TADF (PO-T2T:P1). © Copyright © 2019 Li, Wei, Cao, Fries, Cucchi, Wu, Scholz, Lenk, Voit, Ge and Reineke.
p-Laplace thermistor modeling of electrothermal feedback in organic semiconductors
In large-area Organic Light-Emitting Diodes (OLEDs) spatially inhomogeneous luminance at high power due to inhomogeneous current flow and electrothermal feedback can be observed. To describe these self-heating effects in organic semiconductors we present a stationary thermistor model based on the heat equation for the temperature coupled to a p-Laplace-type equation for the electrostatic potential with mixed boundary conditions. The p-Laplacian describes the non-Ohmic electrical behavior of the organic material. Moreover, an Arrhenius-like temperature dependency of the electrical conductivity is considered. We introduce a finite-volume scheme for the system and discuss its relation to recent network models for OLEDs. In two spatial dimensions we derive a priori estimates for the temperature and the electrostatic potential and prove the existence of a weak solution by Schauder's fixed point theorem.
Reduced Intrinsic Non-Radiative Losses Allow Room-Temperature Triplet Emission from Purely Organic Emitters
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. Results from systematic photophysical investigations, kinetic modeling, excited-state dynamic modeling, and single-crystal structure analysis identify that the long-lived triplets originate from a reduction of intrinsic non-radiative molecular relaxations. Further modification of the N-phenyl ring with halogen atoms affects the afterglow lifetime and quantum yield. As a proof-of-concept, an anticounterfeiting device is demonstrated with a time-dependent Morse code feature for data encryption based on these emitters. A fundamental design principle is outlined to achieve long-lived and emissive triplet states by suppressing intrinsic non-radiative relaxations in the form of molecular vibrations or rotations.
Self-heating, bistability, and thermal switching in organic semiconductors
We demonstrate electric bistability induced by the positive feedback of self-heating onto the thermally activated conductivity in a two-terminal device based on the organic semiconductor C60. The central undoped layer with a thickness of 200 nm is embedded between thinner n-doped layers adjacent to the contacts minimizing injection barriers. The observed current-voltage characteristics follow the general theory for thermistors described by an Arrhenius-like conductivity law. Our findings including hysteresis phenomena are of general relevance for the entire material class since most organic semiconductors can be described by a thermally activated conductivity.
Feel the heat: Nonlinear electrothermal feedback in organic LEDs
For lighting applications, Organic light-emitting diodes (OLED) need much higher brightness than for displays, leading to self-heating. Due to the temperature-activated transport in organic semiconductors, this can result in brightness inhomogeneities and catastrophic failure. Here, we show that due to the strong electrothermal feedback of OLEDs, the common spatial current and voltage distribution is completely changed, requiring advanced device modeling and operation concepts. Our study clearly demonstrates the effect of negative differential resistance (NDR) in OLEDs induced by self-heating. As a consequence, for increasing voltage, regions with declining voltages are propagating through the device, and even more interestingly, a part of these regions show even decreasing currents, leading to strong local variation in luminance. The expected breakthrough of OLED lighting technology will require an improved price performance ratio, and the realization of modules with very high brightness but untainted appearance is considered to be an essential step into this direction. Thus, a deeper understanding of the control of electrothermal feedback will help to make OLEDs in lighting more competitive.
Self-heating effects in organic semiconductor devices enhanced by positive temperature feedback
We studied the influence of heating effects in an organic device containing a layer sequence of n-doped / intrinsic / n-doped C60 between crossbar metal electrodes. A strong positive feedback between current and temperature occurs at high current densities beyond 100 A/cm2, as predicted by the extended Gaussian disorder model (EGDM) applicable to organic semiconductors. These devices give a perfect setting for studying the heat transport at high power densities because C60 can withstand temperatures above 200ʿ C. Infrared images of the device and detailed numerical simulations of the heat transport demonstrate that the electrical circuit produces a superposition of a homogeneous power dissipation in the active volume and strong heat sources localized at the contact edges ...